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Modeling colloid transport for performance assessment.

The natural system is expected to contribute to isolation at the proposed high-level nuclear waste (HLW) geologic repository at Yucca Mountain, NV (YM). In developing performance assessment (PA) computer models to simulate long-term behavior at YM, colloidal transport of radionuclides has been proposed as a critical factor because of the possible reduced interaction with the geologic media. Site-specific information on the chemistry and natural colloid concentration of saturated zone groundwaters in the vicinity of YM is combined with a surface complexation sorption model to evaluate the impact of natural colloids on calculated retardation factors (RF) for several radioelements of concern in PA. Inclusion of colloids into the conceptual model can reduce the calculated effective retardation significantly. Strongly sorbed radionuclides such as americium and thorium are most affected by pseudocolloid formation and transport, with a potential reduction in RF of several orders of magnitude. Radioelements that are less strongly sorbed under YM conditions, such as uranium and neptunium, are not affected significantly by colloid transport, and transport of plutonium in the valence state is only moderately enhanced. Model results showed no increase in the peak mean annual total effective dose equivalent (TEDE) within a compliance period of 10,000 years, although this is strongly dependent on container life in the base case scenario. At longer times, simulated container failures increase and the TEDE from the colloidal models increased by a factor of 60 from the base case. By using mechanistic models and sensitivity analyses to determine what parameters and transport processes affect the TEDE, colloidal transport in future versions of the TPA code can be represented more accurately.

Adsorption↗

Radionuclides in hot mineral spring waters in Jordan.

Hot mineral springs in Jordan are very attractive to people who seek physical healing but they are unaware of natural radioactive elements that may be contained in the hot mineral water. The activities of the natural radioactive isotopes were measured and the concentrations of the parents of their natural radioactive series were calculated. The measured radionuclides were 234Th, 226Ra, 214Pb, 214Bi, 228Ac, 228Th, 212Pb, 212Bi and 208Tl. In addition the activities of 235U and 40K were measured. The activities ranged from 0.14 to 34.8 Bq/l, while the concentrations of parent uranium and thorium isotopes ranged from 3.0 x 10(-3) to 0.59 mg/l. The results were compared with those for drinking water.

Balneology↗

Radioactive discharges from an alkaline pulp mill located in the south of Spain.

Artificial and natural radionuclides present in environmental samples (Eucalyptus wood and bark) can be transferred in an alkaline pulp mill and concentrated in the recycling process. Some part of the radionuclides can be released into the environment associated with the discharges from such a factory. An alkaline pulp mill located in the South of Spain was extensively sampled during 1993 and different radionuclides analysed in the collected samples. Thus the concentrations and fluxes of natural (40K, 226Ra, 228Ra and 228Th) and artificial (137Cs and 90Sr) radionuclides associated with the samples collected along the pulp production process are presented. It is shown that radium and thorium radionuclides behave similarly to strontium and calcium and, consequently, concentrate within the Ca-cycle. Furthermore, 40K and 137Cs are concentrated during the Na-cycle. Finally, the results obtained by the authors are compared with the levels found in similar factories, though situated in the North of Europe, by other researchers.

Environmental Monitoring↗

Contamination of settling ponds and rivers as a result of discharge of radium-bearing waters from Polish coal mines.

Saline waters from underground coal mines in Poland often contain natural radioactive isotopes, mainly 226Ra from the uranium decay series and 228Ra from the thorium series. Approximately 40% of the total amount of radium remains underground as radioactive deposits, but 225 MBq of 226Ra and 400 MBq of 228Ra are released daily into the rivers along with the other mine effluents from all Polish coal mines. Technical measures such as inducing the precipitation of radium in gobs, decreasing the amount of meteoric inflow water into underground workings, etc. have been undertaken in several coal mines, and as a result of these measures, the total amount of radium released to the surface waters has diminished by about 60% during the last 5-6 years. Mine water can have a severe impact on the natural environment, mainly due to its salinity. However, associated high levels of radium concentration in river waters, bottom sediments and vegetation have also been observed. Sometimes radium concentrations in rivers exceed 0.7 kBq/m3, which is the permitted level for waste waters under Polish law. The extensive investigations described here were carried out for all coal mines and on this basis the total radium balance in the effluents has been calculated. Measurements in the vicinity of mine settling ponds and in rivers have given us an opportunity to study radium behaviour in river waters and to assess the degree of contamination. Solid waste materials with enhanced natural radioactivity have been produced in huge amounts in the power and coal industries in Poland. As a result of the combustion of coal in power plants, low-radioactive waste materials are produced, with 226Ra concentration seldom exceeding a few hundreds of Bq/kg. A different situation is observed in coal mines, where, as a result of precipitation of radium from radium-bearing waters, highly radioactive deposits are formed. Sometimes the radioactivity of such materials is extremely high; precipitates from coal mines may have radium concentrations of 400,000 Bq/kg--equivalent to 3% uranium ore. Usually, such deposition takes place underground, but sometimes co-precipitation of radium with barium takes place on the surface, in settling ponds and in rivers. Therefore management of solid waste with technologically enhanced natural radioactivity (TENR) is a very important subject.

Geologic Sediments↗

Abnormal high natural radium concentration in surface waters.

Unexpected high 228Ra concentrations, up to 2 Bq 1(-1), were found in waters of a coastal lagoon close to a monazite sand separation plant. Due to their use as process waters in this plant, the initial supposition was a contamination related to its operation. However, it was concluded that these abnormal radium concentrations had a natural origin, springs at the lagoon head area with high 228Ra and 226Ra concentrations. The strong relationship among radium and light rare-earth elements (LREEs), the observed 228Ra/226Ra activity ratio and the rare-earth element pattern in the spring waters suggested that monazite is the main source of nuclides for water, indicating the disturbance of monazite chemical stability by the combined effects of low pH and high salinity. Both factors combined allow relatively low mobility of thorium, but, on the other hand, a relatively high mobility of radium and LREEs.

Environmental Monitoring↗

Application of multivariate statistical analyses in the interpretation of geochemical behaviour of uranium in phosphatic rocks in the Red Sea, Nile Valley and Western Desert, Egypt.

Factor and cluster analyses as well as the Pearson correlation coefficient have been applied to geochemical data obtained from phosphorite and phosphatic rocks of Duwi Formation exposed at the Red Sea coast. Nile Valley and Western Desert. Sixty-six samples from a total of 71 collected samples were analysed for SiO2, TiO2, Al203, Fe2O3, CaO, MgO, Na2O, K2O, P2O5, Sr, U and Pb by XRF and their mineral constituents were determined by the use of XRD techniques. In addition, the natural radioactivity of the phosphatic samples due to their uranium, thorium and potassium contents was measured by gamma-spectrometry. The uranium content in the phosphate rocks with P2O5 > 15% (average of 106.6 ppm) is higher than in rocks with P2O5 < 15% (average of 35.5 ppm). Uranium distribution is essentially controlled by the variations of P2O5 and CaO, whereas it is not related to changes in SiO2, TiO2, Al2O3, Fe2O3, MgO, Na2O and K2O concentrations.-Factor analysis and the Pearson correlation coefficient revealed that uranium belaves geochemically in different ways in the phosphatic sediments and phosphorites in the Red Sea, Nile Valley and Western Desert. In the Red Sea and Western Desert phosphorites, uranium occurs mainly in oxidized U6+ state where it seems to be fixed by the phosphate ion, forming secondary uranium phosphate minerals such as phosphuranylite. In the Nile Valley phosphorites, ionic substitution of Ca2+ by U4 is the main controlling factor in the concentration of uranium in phosphate rocks. Moreover, fixation of U6- by phosphate ion and adsorption of uranium on phosphate minerals play subordinate roles.

Egypt↗

Evaluation of technologically enhanced natural radiation near the coal-fired power plants in the Lodz region of Poland.

Radionuclide releases together with escaping fly ashes (from 45 x 10(6) kg in previous decades to 8 x 10(6) kg annually in 1996) from the main local and several small coal-fired power plants resulted in a relatively small increase in natural radioactivity levels in the Lodz region. The natural gamma terrestrial radiation dose rates (1 m above ground level) were measured at 82 points including in the vicinity of power plants, in the center of the town and on edge of the town. The average dose rate value for the first area was 36 +/- 1.2 nGy h (-1), whereas the same dose rate for the edge of town was slightly lower 30 +/- 0.9 nGy h (-1) but this difference was statistically significant. Further confirmation of the technologically slightly enhanced exposure of the local population to natural radionuclides was achieved by gamma-spectrometry measurement of the uranium and thorium decay series radionuclides in the surface soil profiles (up to 30 cm depth). The average increase of 226Ra and 232Th radionuclides in the top layer of soil (0-10 cm) according to the 20+/-30 cm depth layer was 21% and 17%, respectively. However, due to the relatively low levels of 232Th (14.3 Bq kg (-1)) and 238U (16.8 Bq kg (-1)) in this area, the annual average effective dose from the natural terrestrial radiation for the local population is also relatively low, 0.28 mSv only.

Coal↗

Radon flux at King George Island, Antarctic Peninsula.

Fluxes of 222Rn from the ice-free terrain to the atmosphere were measured directly, for the first time, at the Brazilian Antarctic Station Ferraz during the summer field campaign of 1998/99. Average value for the flux was 7.7 +/- 4.8 x 10(-2) atoms cm(-2) s(-1) and it ranged between 0.21 x 10(-2) atoms cm(-2) s(-1) and 28 x l0(-2) atoms cm(-2) s(-1). The average flux of 220Rn was estimated to be 23 atoms cm(-2) s(-1), using a combination of two techniques: nuclear track detection and alpha spectrometry of radon daughters. It was found that the production of radon by uranium (41.54 + /-7.17 Bq kg(-1)) and thorium (57.97 +/- 12.14 Bq kg(-1)) equivalent soil contents, and a diffusion coefficient derived from experimental data for the local terrain could account for this average flux. Nevertheless, the large surges of 222Rn in the atmosphere frequently observed for that area could not be explained by this flux only.

Antarctic Regions↗

The influence of urbanization on natural radiation levels in anomalous areas.

This paper verifies the effects of urbanization on the original levels of environmental gamma radiation in an anomalous area. The fieldwork was done in the city of Guarapari, on the seacoast of the state of Espírito Santo, Brazil. This place was chosen because the whole region is naturally rich in monazite sand, which contains thorium and uranium. A similar study was also carried out in the 1960s. The measurements were done using an inorganic NaI scintillometer detector with Cu+Pb filters coupled to a scaler. The methodology of measurements used was similar to the one applied in the fieldwork carried out in the 1960s. In addition, a simulation was performed in the laboratory, to determine the attenuation of the materials used in the urbanization of the region. The results of this work clearly show that there was a reduction in the levels of external radiation in the streets and squares of Guarapari. It was concluded that the reduction was due to attenuation by the materials used in the urbanization.

Background Radiation↗

The influence of a coal-fired power plant operation on radionuclide concentrations in soil.

Fifty-two soil samples in the vicinity of a coal-fired power plant (CFPP) in Figueira (Brazil) were analyzed. The radionuclide concentration for the uranium and thorium series in soils ranged from <9 to 282 Bq kg(-1). The range of 40K concentration in soils varied from <59 to 412 Bq kg(-1). The CFPP (10 MWe) has been operating for 35 years and caused a small increment in natural radionuclide concentration in the surroundings. This technologically enhanced natural radioactivity (TENR) was mainly due to the uranium series (234Th, 226Ra and 210Pb) and was observable within the first kilometer from the power plant. The CFPP influence was only observed in the 0-25 cm soil horizon. The soil properties prevent the radionuclides of the 238U-series from reaching deeper soil profiles. The same behavior was observed for 40K as well. No influence was observed for 232Th, which was found in low concentrations in the coal.

Coal↗

Radiographic findings in 224Ra-caused dental resorptions.

Dental resorptions as a delayed effect of Thorium X (224Ra) were observed in four patients. The radiographic findings showed distinct and representative patterns. Apparently, the observed changes are typical for delayed alterations related to 224Ra-specific disturbances in the alveolar process. Degenerative and inflammatory reactions may also be involved in the pathogenesis.

Adult↗

Selective removal of plutonium 238 from a canal sediment using a carbonate-chelant soil washing technology (ACT*DE*CON).

The Mound laboratory site in Miamisburg, OH, a former plutonium processing facility, contains approximately 40000 yd(3) (30,580 m3) of plutonium- and thorium-contaminated soils and sediments at levels that require remediation. Existing applicable remediation technologies are unsatisfactory, because they are expensive and do not provide volume reduction. ACT*DE*CON is a chemical soil leaching technology for the treatment of soils that utilizes contaminant dissolution via dilute selective solutions to remove radionuclides. In bench-scale tests, process parameters were developed for the optimal treatment of the Miami Erie Canal soil at the Mound site, combining the maximum plutonium removal with an acceptable amount of soil dissolution and minimizing the costs of reagents. Parameters evaluated included soil to extractant mass ratio, temperature, rinse solution composition, kinetics, and the application of several dewatering aids. Plutonium removal rates of >95% were achieved, and the residual plutonium in the treated soil proved to be very immobile-confirming that the process had removed the most accessible species of the radionuclide. Currently being tested at Mound is an engineering scale-up that includes an attrition scrubber, a counter-current extractor, and a reverse osmosis system. Economic evaluations based on bench-scale results put the treatment cost at US$278/yd(3) (US$364/m3), compared to US$350/yd(3) (US$458/m3) for the 'box-and-bury' baseline alternative treatment system.

Carbonates↗

ESR study of elephant tooth enamel from the Kärlich-Seeufer site in Germany.

Enamel from 6 different positions in a well preserved elephant tooth from the Kärlich-Seeufer site in Germany has been irradiated up to 32 kGy. The X-band (v = 9.5 GHz) ESR spectra of two subsamples have been decomposed into three real components with Maximum Likelihood Common Factor Analysis (MLCFA). One of these components due to orthorhombic CO2- radicals is predominant. Dose response curves for the contributions of these MLCFA components and for different heights in the ESR spectra have been obtained and fitted with different models. Depending on the model, the equivalent dose for the preferably used height at g = 1.9973, due to CO2-, ranges from 70 to 130 Gy. Due to a very low uranium and thorium content in both enamel and dentine (< or = approximately 10 ppb) and to an important external y-attenuation, the ages fluctuate between 300 and 575 ka.

Animals↗

The standardisation of 229Th for an environmental yield tracer

The naturally occurring long-lived nuclides of thorium (228Th, 230Th and 232Th) are all alpha-emitters that are of interest both to the nuclear and non-nuclear industries and levels of these nuclides need to be monitored in both the working and natural environment. In order to do this in a manner where the results of radiochemical analysis are traceable to national standards, a chemical yield tracer has to be employed. 229Th has been identified as a suitable tracer for such purposes and has been used in the past. This paper describes the absolute standardisation of 225Th by 47pi alpha-gamma coincidence counting. The results of this work are presented together with an analysis of the standardisation uncertainties that were achieved in practice.

Journal Article↗

Coincidence summing corrections for the natural decay series in gamma-ray spectrometry.

Using a Monte Carlo code and a Markov formalism to describe the decay schemes, coincidence-summing correction factors can be calculated with a suitable accuracy. For two different measuring geometries and an HPGe detector, calculated and experimental correction factors have been shown to closely agree for 152Eu. The simulation method has subsequently been applied in assessing the need for coincidence-summing corrections for members of the uranium, thorium and actinium series measurable by gamma-spectrometry. Correction factors were calculated for predominant gamma emissions significantly affected by coincidence-summing effects and the correctness of our calculations tested for environmental samples. The test makes it evident that in order to obtain reliable and unbiased activity values for some natural radionuclides coincidence summing cannot be neglected in environmental measurements at small source-detector distances.

Journal Article↗

Minimum detectable activity in in situ gamma-ray spectrometry.

The algorithm used to calculate a minimum detectable activity (A(D)) of an environmental volume sample measured by gamma-ray spectrometry was modified and adapted for in situ measurements performed at the standard 1 m height above ground. AD values of target radionuclides were determined from the in situ spectra collected at two disparate sites. A linear relationship between the two sets of A(D)s was found and the ratio between these two sets is equal to the square root of the ratio of the two respective absorbed dose rates measured at the sites at 1 m height. Absorbed dose rates were calculated using the concentration of potassium, thorium and uranium in the soils at the sites and found to agree well with the measured values. A(D) values can be predicted easily in in situ gamma spectrometry applying a simple experimental procedure that is based on the linear relationship.

Journal Article↗

A new method for evaluating radon and thoron alpha-activities per unit volume inside and outside various natural material samples by calculating SSNTD detection efficiencies for the emitted alpha-particles and measuring the resulting track densities.

A Monte Carlo computer code for determining detection efficiencies of the CR-39 and LR-115 II solid-state nuclear track detectors (SSNTD) for alpha-particles emitted by the uranium and thorium series inside different natural material samples was developed. The influence of the alpha-particle initial energy on the SSNTD detection efficiencies was investigated. Radon (222Rn) and thoron (220Rn) alpha-activities per unit volume were evaluated inside and outside the natural material samples by exploiting data obtained for the detection efficiencies of the SSNTD utilized for the emitted alpha-particles, and measuring the resulting track densities. Results obtained were compared to those obtained by other methods. Radon emanation coefficients have been determined for some of the considered material samples.

Algorithms↗

Plutonium oxidation states in seawater.

Studies of the oxidation-state distribution of plutonium in the ocean illustrate the need to characterize seawater by means of the pH, the E(H), and quanititative complexation parameters. The parameters are combined in an easy-to-use equation that determines the fractions of the four oxidation states. Similar analyses have been applied to plutonium in other solutions, and the same methods can be applied to seawater. An appendix shows how to estimate and interpret the alpha coefficient for tetravalent plutonium using published information for tetravalent thorium.

Journal Article↗