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Leaching characteristics of paraffin waste forms generated from Korean nuclear power plants.

Leaching tests of paraffin waste forms including boric acid, cobalt, strontium and cesium were performed to investigate the leaching characteristics of paraffin waste forms which had been generated in Korean nuclear power plants. The leaching tests were conducted according to ANSI/ANS-16.1 test procedure and the cumulative fractions leached (CFLs) of boric acid, cobalt, strontium and cesium were obtained. The compressive strength before and after the leaching test was measured for various waste forms with different mixing ratios of boric acid to paraffin. It was observed that boric acid and other nuclides immobilized within paraffin waste forms were congruently released and the leaching rates were influenced by reacted layer depth as the dissolution reaction progressed. A shrinking core model based on the diffusion-controlled dissolution kinetics was developed in order to simulate the test results. The CFLs and the leaching rates were well expressed by the shrinking core model and the cross-sectional view of specimen after the test demonstrated the applicability of this model with the shrinking dissolution front to the leaching analysis of paraffin waste forms.

Boric Acids↗

Leaching of depleted uranium in soil as determined by column experiments.

The basic features of the leachability of depleted uranium (DU) projectiles in soil was investigated by using 12 projectiles (145-294 g DU) and 16 columns installed in an air-conditioned laboratory. Two soils widely distributed in Europe, a sandy-loamy cambisol and a silty-loamy luvisol, were filled into the columns (3.3 kg dry soil each). The effluents of all columns were collected weekly during the observation period of 1 year. In 648 samples, 235U and 238U were determined by inductively coupled plasma mass spectrometry. The leaching rates of 238U from natural uranium were in general about 0.01 microg week-1 or smaller, while those of 238U from the DU munitions varied considerably and reached values of up to 100 microg week-1, for the different columns. In total, about 0.3 microg natural uranium corresponding to 20 ppm of its inventory in the soil was leached during the observation period. From the projectiles, an average of about 50 microg DU were leached corresponding to 18 ppm of the corroded DU mass (about 1.6% of the mean initial DU mass of the projectiles). Assuming that corrosion and leaching continue as observed, the mobilisation of 238U from DU munitions will last, on an average, for thousands of years in the soils investigated, while the munitions themselves will have been corroded after a much shorter time. It is proposed to use, for the investigated soil types, the mean leaching rates of the six columns with projectiles for transport calculations of 238U to the groundwater and, thus, for a better risk assessment of the water-dependent uptake pathways of DU.

Diffusion↗

Influence of the colloid type on the transfer of 60Co and 85Sr in silica sand column under varying physicochemical conditions.

The influence of two types of colloids (natural organic matter, NOM), a colloid with high affinity for radionuclides (RN(s)), and hydrophilic synthetic latex (SHL), a colloid with low affinity for RN(s) on the transfer of (60)Co and (85)Sr in a silica sand column was studied under different physicochemical conditions: pH (4.9), ionic strength (10(-3) M and 10(-2) M), concentration of colloids (100 mg l(-1), 10 mg l(-1)), flow velocity (12.4 cm h(-1) and 3.7 cm h(-1)), water saturation of the column (100% and 70%). In the absence of colloids, the transfer of (60)Co and (85)Sr was retarded compared to the transfer of the conservative tracer. In the presence of colloids and according to the specific physicochemical conditions, an acceleration or retardation of (60)Co and (85)Sr transfer was observed compared to their transfer in the absence of colloids. Our results evidenced that any colloids even with low reactivity could significantly modify the RN transfer. However, the extent to which the transfer was influenced differs according to the colloid type; the NOM exhibiting higher impact than SHL. Batch experiments helped in interpreting of the interactions between the colloids, RN(s) and solid phase observed in column.

Cobalt Radioisotopes↗

Soil to plant transfer of 238U, 226Ra and 232Th on a uranium mining-impacted soil from southeastern China.

Both soil and plant samples of nine different plant species grown in soils from southeastern China contaminated with uranium mine tailings were analyzed for the plant uptake and translocation of 238U, 226Ra and 232Th. Substantial differences were observed in the soil-plant transfer factor (TF) among these radionuclides and plant species. Lupine (Lupinus albus) exhibited the highest uptake of 238U (TF value of 3.7x10(-2)), while Chinese mustard (Brassica chinensis) had the least (0.5x10(-2)). However, in the case of 226Ra and 232Th, the highest TFs were observed for white clover (Trifolium pratense) (3.4x10(-2)) and ryegrass (Lolium perenne) (2.1x10(-3)), respectively. 232Th in the tailings/soil mixture was less available for plant uptake than 226Ra or 238U, and this was especially evident for Chinese mustard and corn (Zea mays). The root/shoot (R/S) ratios obtained for different plants and radionuclides shown that Indian mustard had the smallest R/S ratios for both 226Ra (5.3+/-1.2) and 232Th (5.3+/-1.7), while the smallest R/S ratio for 238U was observed in clover (2.8+/-0.9).

China↗

Distribution and sources of (129)I in rivers of the Baltic region.

The concentration of (129)I was measured in 54 river waters discharging into the Baltic Sea from Sweden, Finland, Estonia, Latvia, Lithuania, Poland and Germany. Sample collection was performed during a well-bracketed time interval (June-July 1999), thus allowing comparison of the rivers over a wide latitude range without the effect of long temporal spread. Although there is no direct input of anthropogenic (129)I in the watersheds, the concentration of the isotope is about two to three orders of magnitude higher than the expected pre-nuclear era natural values in the rivers of Finland and northern Sweden, and in the rivers of southern Sweden, Lithuania, Estonia, Latvia, Poland and Germany; the (129)I concentration may reach five orders of magnitude higher. Furthermore, there are significant correlations between the (129)I concentration and latitude and/or distance from the North Sea and between (129)I and Cl. These findings suggest seawater as a main source of (129)I to the rivers through atmospheric transport. Of the many chemical parameters investigated, the pH may account for some of the variability in (129)I concentrations of the rivers. The contribution from nuclear weapon tests and the Chernobyl accident to the riverine (129)I is insignificant compared to the releases from the nuclear fuel reprocessing facilities. The total flux of (129)I by rivers to the Baltic Sea and related basins represents minor amounts of the isotope pool in these marine waters. External radioactivity hazards from (129)I are considered to be negligible in the Baltic region. However, as the main (129)I intake to the human body is likely through water, due to the large amount of daily water consumption, more concern should be given to internal radioactivity hazard that may be associated with the isotope's localized elevated concentration in the human organs.

Baltic States↗

A methodology for the assessment of rehabilitation success of post mining landscapes--sediment and radionuclide transport at the former Nabarlek uranium mine, Northern Territory, Australia.

Protection of the environment post-mining is an important issue, especially where runoff and erosion can lead to undesirable material leaving post-mining landscapes and contaminating surrounding land and watercourses. Methods for assessment of the environmental impact and long-term behaviour of post-mining landforms based on scientific methodology are needed especially where field data are absent or poor. An appraisal of the former Nabarlek uranium mine was conducted to assess the site from a soil erosion perspective as part of an independent evaluation of overall rehabilitation success. Determination of the gross erosion occurring, sediment discharge to Cooper Creek and the resultant sediment associated radionuclide load in Cooper Creek were the primary objectives of the study. These objectives were achieved through the application of several models using parameter values collected from the site. The study found that the area containing the mill tailings repository is extremely stable and meets the guidelines established for long-term storage of uranium mill tailings. Most other areas on the site are stable; however there are some areas with a high sediment loss. Sediment concentration in Cooper Creek, which drains the site, was found to be within the Australian water quality guidelines for fresh water, however sediment concentrations in tributaries were found to exceed recommended levels. Radionuclide determinations on soil samples showed that the highest specific activities (Bq kg-1) were present on a small (0.44 ha) area with a relatively high erosion rate. This small area contributed the majority of the estimated flux to Cooper Creek of uranium-series radionuclides sorbed or structurally incorporated to eroded soil particles sourced from the mine site. This study provides a methodology for assessment of the erosional stability of such a landscape and consequent impact on water quality, using extensive field data and readily available and well known models and methodologies.

Environmental Monitoring↗

Experimental and modeling studies on sorption and diffusion of radium in bentonite.

The sorption and desorption behavior of radium on bentonite and purified smectite was investigated as a function of pH, ionic strength and liquid to solid ratio by batch experiments. The distribution coefficients (Kd) were in the range of 10(2) to > 10(4) ml g-1 and depended on ionic strength and pH. Most of sorbed Ra was desorbed by 1 M KCl. The results for purified smectite indicated that Ra sorption is dominated by ion exchange at layer sites of smectite, and surface complexation at edge sites may increase Ra sorption at higher pH region. Reaction parameters between Ra and smectite were determined based on an interaction model between smectite and groundwater. The reaction parameters were then used to explain the results of bentonite by considering dissolution and precipitation of minerals and soluble impurities. The dependencies of experimental Kd values on pH, ionic strength and liquid to solid ratio were qualitatively explained by the model. The modeling result for bentonite indicated that sorption of Ra on bentonite is dominated by ion exchange with smectite. The observed pH dependency was caused by changes of Ca concentration arising from dissolution and precipitation of calcite. Diffusion behavior of Ra in bentonite was also investigated as a function of dry density and ionic strength. The apparent diffusion coefficients (Da) obtained in compacted bentonite were in the range of 1.1 x 10(-11) to 2.2 x 10(-12) m2 s-1 and decreased with increasing in dry density and ionic strength. The Kd values obtained by measured effective diffusion coefficient (De) and modeled De were consistent with those by the sorption model in a deviation within one order of magnitude.

Adsorption↗

Potential remobilization of 137Cs, 60Co, 90Tc, and 90Sr from contaminated Mayak sediments in river and estuary environments.

Following 50 years of nuclear production at Mayak PA, sediments in storage reservoirs are significantly contaminated. Dam failure or flooding could potentially transport large amounts of sediments, via rivers, to the Ob estuary and Kara Sea. The objectives of this work were to investigate fresh and seawater remobilization of 137Cs, 50Co, 99Tc, and 90Sr from contaminated Reservoir 10 sediments. Sediments were extracted sequentially using synthetic Techa freshwater, seawater, and chemical reagents with increasing dissolution powers. 137Cs and 90Sr freshwater distribution coefficients (apparent Kd) agreed quite well with published values; values for 99Tc were higher and values for 60Co were lower than expected. In seawater, mean apparent Kd values decreased by 94, 77, 48, and 73% (137Cs, 60Co, 99Tc, and 90Sr, respectively), indicating increased radionuclide mobility. Remobilization in seawater was 5, 15, 1, and 23% of total activities (i.e., releases of 165, 11, 0.3, and 170 kBq kg(-1) d.w.) for 137Cs, 60Co, 99Tc, and 90Sr, respectively. 137Cs and 99Tc were strongly bound to sediments (60% and 80%, respectively). 60Co and 90Sr were more mobile (70% reversibly bound). In conclusion, Mayak Reservoir sediments could potentially contaminate the Ob estuary due to remobilization of sediment-held radionuclides upon contact with seawater.

Environmental Monitoring↗

Decommissioning of a nuclear power plant: determination of site-specific sorption coefficients for Co-60 and Cs-137.

Assessment of radiological risks in strategies for decommissioning of nuclear installations have to consider not only technical concepts such as cutting and decontamination techniques but, even more important, requirements for input of reliable information on the hydrological situation and retardation capabilities of relevant radionuclides specific to the respective decommissioning operation. In this paper we describe appropriate methods for obtaining site-specific sorption data and present results achieved from a case study performed as a commercial contractual work preliminary to the planned decommissioning of a nuclear power plant. A detailed mineralogical study of the sediment used in our sorption experiment highlights the necessity of a thorough sample homogenization and characterization. Batch experiments using radiotracer techniques for the determination of site-specific sorption coefficients show significant retardation for Co-60 and Cs-137 after only 2 h of equilibration between the preconditioned groundwater and sediment. Sorption is more effective in the groundwater of a deeper aquifer containing a higher amount of colloidal clay (illite) particles < 0.63 micron. The Co-60 radiotracer is more completely sorbed than the Cs-137 radiotracer. Equilibration of radionuclide distribution is slow, particularly for Co-60. Presence of EDTA reduces sorption of Co-60 efficiently while Cs-137 sorption remains unaffected.

Adsorption↗

Modelling the contribution of individual radionuclides to the total gamma air kerma rate for the sediments of the Ribble Estuary, NW England.

The aim of this study was to test the performance of a published dose-rate model, investigate the contribution of individual radionuclides to the total gamma air kerma rate (GAKR) and derive external doses to man in the Ribble Estuary, NW England. GAKRs were measured and sediment cores were collected in order to determine radionuclide specific activities with depth. The latter values were used as input data for the external dose-rate model. The model has a slight tendency to over-predict the GAKR, but, on average, the model predictions fall within +/-26% of the measured value. Improvements, in the present case, might be made by accounting for core shortening and variations in soil density in the input data. The model predicted that, for exposed intertidal mud sites, a range of GAKRs between 0.011 and 0.022 microGy h(-1) was attributable to Springfields discharges alone. The contribution due to 234mPa and 234Th ranged between 20 and 60%. An excess GAKR (GAKR arising from anthropogenic emissions alone) of 0.139-0.150 microGy h(-1), used in conjunction with relevant habit-survey data (for a potential critical group) and conversion factors, yielded a dose to man of 0.029-0.031 mSv year(-1).

Air Pollutants, Radioactive↗

Investigations of thermoluminescence dosimetry in the Techa river flood plain: analysis of the new results.

The Techa river region was highly contaminated due to radioactive releases from a nuclear production facility in the period from 1949 to 1956. The inhabitants of the upper Techa river settlements received significant doses of external radiation. The majority of the houses in the upper Techa river villages were demolished after the evacuation of the population in 1956. Only three buildings (red-brick construction) in the former village of Metlino can still be used for thermoluminescence (TL) investigations in an external dose reconstruction study. The radiation source configuration changed in 1956 after an artificial reservoir was created next to Metlinsky pond. Preliminary TL studies showed good properties of the bricks that were sampled from the buildings. This paper presents an analysis of new results of TL investigations obtained on the samples collected from different walls of the buildings. The highest dose values in the range 1-4 Gy were found in bricks collected from the walls of building exposed to the artificial reservoir (Reservoir-10) and values of 1-1.5 Gy were found next to the Metlinsky pond shoreline. The measurements of the radiation source geometry were carried out simultaneously with the dose rates, radionuclide concentration in water and bottom sediments near the wall facing the old river bed. The measurements allow a validation of models used in the current Techa River Dosimetry System (TRDS-2000) to estimate external doses of the former inhabitants of the upper Techa riverside. In particular, the results can be applied for a more correct description of the source geometry in the settlement.

Fresh Water↗