A study of radionuclides, metals and stable lead isotope ratios in sediments and soils in the vicinity of natural U-mineralisation areas in the Northern Territory

Australian guidelines recommend that tailings materials from uranium (U) mining and milling be contained without any detrimental impact on the environment for at least 1000 years. Natural analogue sites are being investigated to determine if they can provide data on the rates of natural erosion processes which occur over these timescales, for input into predictive geomorphic computer models. This paper presents radionuclide, metal and stable lead (Pb) isotope data from sediment cores and surface soils in the vicinity of two mineralised areas in the Alligator Rivers Region.Surface scrapes from the natural Anomaly #2, south of the Ranger mineral lease, exhibit radiogenic ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁷Pb ratios, and elevated U and metal concentrations typical for a near surface U anomaly. In contrast, samples taken from the Koongarra mineral lease (KML) show radionuclide activity and metal concentrations similar to natural areas elsewhere in the Alligator Rivers Region and Pb isotope ratios are closer to present day average crustal ratios (PDAC), as the orebodies at KML are covered by surficial sand. A sediment core collected from Anbangbang Billabong, downstream of KML, exhibits small variations in Pb isotope ratios that indicate that approximately 1% of the upper sediments in the sediment core may be derived from material originating from the U anomaly at Koongarra.     

The effects of <Emphasis Type="Italic">Acidithiobacillus ferrooxidans</Emphasis> on the leaching of cobalt and strontium adsorbed onto soil particles

Bioleaching from soil artificially contaminated with analogues of radionuclides, Co and Sr, was carried out using a Fe-oxidizing bacterium, Acidithiobacillus ferrooxidans. Due to bacterial metabolism, the pH and dissolved Fe³⁺ concentration in a biotic slurry decreased and increased respectively, over time, but the concentrations of Co and Sr extracted from the soil showed no significant enhancement compared with those under abiotic control. In both cases, Co and Sr were leached from the soil during the initial period of the experiment, due to the initially low solution pH of 2.0, and the dissolved concentrations remained almost constant for the duration of the experiment (300 h). Since oxidation of Fe²⁺ by A. ferrooxidans led to the production of Fe precipitates and colloidal suspensions, the Co and Sr extracted into solution were most likely re-adsorbed onto the Fe solids. Also, A. ferrooxidans, without an external supply of Fe²⁺, extracted almost equal or greater amounts of Co and Sr from the soil than when Fe²⁺ was supplied. Under the same leaching conditions, the extent of Sr removal was much lower than that of Co. On the contrary to the high efficiency of microbial metal leaching in biohydrometallurgy for low-graded sulfide ores, which has been widely documented, conventional bioleaching techniques with A. ferrooxidans supplied with enough Fe²⁺ showed low efficiency for the removal of radionuclides loosely bound onto soil particle surfaces.     

Chemistry, mineralogy and radioactivity in posidonia oceanica meadows from North-Western Sicily

This paper presents measurements of major, minor, metal trace elements and radionuclides in sediments and in Posidonia oceanica samples from north-western Sicily (Italy). The mineralogical and chemical composition of sediments were determined by X-ray diffraction and X-ray fluorescence techniques, respectively. A flame atomic absorption spectrophotometry was used to measure concentrations of Cu, Zn, Cd and Pb in P. oceanica samples and in sediments. Specific activities of selected radionuclides have been determined by high-resolution gamma spectrometry. Standard statistical analysis was used to assess correlations between different elements and different sample types.     

Solute transport properties of compacted Ca-bentonite used in FEBEX project

The present Spanish concept of a deep geological high level waste repository includes an engineered clay barrier around the canister. The clay presents a very high sorption capability for radionuclides and a very small hydraulic conductivity, so that the migration process of solutes is limited by sorption and diffusion processes. Therefore, diffusion and distribution coefficients in compacted bentonite (i.e. in "realistic" liquid to solid ratio conditions) are the main parameters that have to be obtained in order to characterise solute transport that could be produced after the canister breakdown. Through-Diffusion (TD) and In-Diffusion (ID) experiments with HTO, Sr, Cs and Se were carried out using compacted FEBEX bentonite, which is the reference material for the Spanish concept of radioactive waste disposal. Experiments were interpreted by means of available analytical solutions that allow the estimation of diffusion coefficients and, in some cases, distribution coefficients. Analytical solutions are simple to use, but rely on hypotheses that do not hold in all the experiments. These experiments were interpreted also using an automatic parameter estimation code that overcomes the limitations of analytical solutions. Numerical interpretation allows the simultaneous estimation of porosity, diffusion and distribution coefficients, accounts for the role of porous sinters and time-varying boundary concentrations, and can use different types of raw concentration data.     

Sensitivity analysis of radionuclide migration in compacted bentonite: a mechanistic model approach

Mechanistic model calculations for the migration of Cs, Ra, Am and Pb in compacted bentonite have been carried out to evaluate sensitivities with respect to different parameter variations. A surface chemical speciation/electric double layer model is used to calculate: (i) porewater composition and radionuclide speciation in solution and at the bentonite surface, yielding the distribution of mobile and sorbed species and (ii) interaction of diffusing species with negatively charged pore walls to obtain diffusion parameters. The basic scenario considers the interaction of compacted bentonite with a fresh-type groundwater; variations include the presence of bentonite impurities and saline groundwater. It is shown that these scenarios result in significant variations of porewater composition that affect migration via three mechanisms that can partly compensate each other: (1) effects on sorption through radionuclide complexation in solution, and competition of major cations for surface sites; (2) changes in radionuclide solution speciation leading to different diffusing species under different conditions; (3) effects on diffusion through changes in the electric double layer properties of the clay pores as a function of ionic strength.     

Cesium-137 monitoring using mosses from W. Macedonia,N. Greece

¹³⁷Cs activities in mosses and substrate (soil, bark) collected from W. Macedonia, Greece were measured 20 years after the Chernobyl reactor accident. Archive material from previous studies was also used for comparison and diachronic estimation of the radio-contamination status. A gradual decrease was detected which depended on various factors such as the collected species, location, growth rate and substrate. Maximum accumulation capacity of ¹³⁷Cs was observed in the epilithic mosses in comparison to the epiphytic ones. The ¹³⁷Cs content in the bark of the two broad-leaved species (oak and fagus) was higher than that of the conifer (pinus). Bark specimens of about 50 cm height were in general more contaminated than those of 200 cm. Autoradiography revealed an amount of ¹³⁷Cs distributed more or less uniformly in moss thalli. The high ¹³⁷Cs activities found in mosses 20 years after Chernobyl suggest that these primitive plants are effective, suitable and inexpensive biological detectors of the distribution and burden of radionuclide fallout pattern.     

Cesium and strontium sorption by selected tropical and subtropical soils around nuclear facilities

The dynamics of Cs and Sr sorption by soils, especially in the subtropics and tropics, as influenced by soil components are not fully understood. The rates and capacities of Cs and Sr sorption by selected subtropical and tropical soils in Taiwan were investigated to facilitate our understanding of the transformation and dynamics of Cs and Sr in soils developed under highly weathering intensity. The Langmuir isotherms and kinetic rates of Cs and Sr sorption on the Ap1 and Bt1 horizons of the Long-Tan (Lt) and the A and Bt1 horizons of the Kuan-Shan (Kt), Mao-Lin (Tml) and Chi-Lo (Cl) soils were selected for this study. Air-dried soil (<2 mm) samples were reacted with of 7.5 × 10⁻⁵ to 1.88 × 10⁻³ M of CsCl (pH 4.0) or 1.14 × 10⁻⁴ to 2.85 × 10⁻³ M of SrCl₂ (pH 4.0) solutions at 25 °C. The sorption maximum capacity (q_m) of Cs by the Ap1 and Bt1 horizons of the Lt soil (62.24 and 70.70 mmol Cs kg⁻¹ soil) were significantly (p < 0.05) higher than those by the A and Bt1 horizons of the Kt and Cl soils (26.46 and 27.49 mmol Cs kg⁻¹ soil in Kt soil and 34.83 and 29.96 mmol Cs kg⁻¹ soil in Cl soil, respectively), however, the sorption maximum capacity values of the Lt and Tml soils did not show significant differences. The amounts of pyrophosphate extractable Fe (Fe_p) were correlated significantly with the Cs and Sr sorption capacities (for Cs sorption, r² = 0.97, p < 1.0 × 10⁻⁴; for Sr sorption, r² = 0.82, p < 2.0 × 10⁻³). The partition coefficient of radiocesium sorbed on soil showed the following order: Cl soil ? Kt soil > Tml soil > Lt soil. It was due to clay minerals. The second-order kinetic model was applied to the Cs and Sr sorption data. The rate constant of Cs or Sr sorption on the four soils was substantiality increased with increasing temperature. This is attributable to the availability of more energy for bond breaking and bond formation brought about by the higher temperatures. The rate constant of Cs sorption at 308 K was 1.39-2.09 times higher than that at 278 K in the four soils. The activation energy of Cs and Sr sorbed by the four soils ranged from 7.2 to 16.7 kJ mol⁻¹ and from 15.2 to 22.4 kJ mol⁻¹, respectively. Therefore, the limiting step of the Cs⁺ or Sr²⁺ sorption on the soils was diffusion-controlled processes. The reactive components, which are significantly correlated with the Langmuir sorption maxima of Cs and Sr by these soils, substantially influenced their kinetic rates of Cs and Sr sorption. The data indicate that among components of the subtropical and tropical soils studied, short-range ordered sesquioxides especially Al- and Fe-oxides complexed with organics play important roles in influencing their capacity and dynamics of Cs and Sr sorption.     

Model reduction via principal component truncation for the optimal design of atmospheric monitoring networks

A numerically efficient methodology for the optimal design of monitoring networks aiming at the surveillance of accidental atmospheric release is proposed in this paper. In a realistic context, the design of such a network requires the knowledge of a database of potential dispersion accidents occurring in the domain of the study. An objective function measures the ability of a potential network to provide measurements in order to reconstruct any accidental plume taken from the database. In the optimisation of such cost functions with respect to networks, most of the computational time is spent in the evaluation of the function, especially if the accidents database is large. In this paper we show how to optimally reduce this database and how this affects the design via a mathematical expansion in the cost function. We introduce methods based on principal component analysis, which are rigorous when the cost function is of least-squares type. These methods are then tested and validated with success on the design of a radionuclides monitoring network to be deployed over France. This is the so-called Descartes network which will be operated by the French Institute for Radiation and Nuclear Safety. These techniques are then applied on Descartes to solve several issues that are computationally demanding, but are also of more general interest, such as: how should one sequentially deploy the stations of the network? How is affected the optimal network when other European potential radiological sources are taken into account?     

Scientific research, stakeholders, and policy: continuing dialogue during research on radionuclides on Amchitka Island, Alaska

It is increasingly clear that a wide range of stakeholders should be included in the problem formulation phase of research aimed at solving environmental problems; indeed the inclusion of stakeholders at this stage has been formalized as an integral part of ecological risk assessment. In this paper, we advocate the additional inclusion of stakeholders in the refinement of research methods and protocols and in the execution of the research, rather than just at the final communication and reporting phase. We use a large study of potential radionuclide levels in marine biota around Amchitka Island as a case study. Amchitka Island, in the Aleutian Island Chain of Alaska, was the site of three underground nuclear tests (1965-1971). The overall objective of the biological component of the study was to collect a range of marine biota for radionuclide analysis that could provide data for assessing current food safety and provide a baseline for developing a plan to monitor human and ecosystem health in perpetuity. Stakeholders, including regulators (State of Alaska), resource trustees (US Fish and Wildlife Service, State of Alaska), representatives of the Aleut and Pribilof Island communities, the Department of Energy (DOE), and others, were essential for plan development. While these stakeholders were included in the initial problem formulation and approved science plan, we also included them in the refinement of protocols, selection of bioindicators, selection of a reference site, choice of methods of collection, and in the execution of the study itself. Meetings with stakeholders resulted in adding (or deleting) bioindicator species and tissues, prioritizing target species, refining sampling methods, and recruiting collection personnel. Some species were added because they were important subsistence foods for the Aleuts, and others were added because they were ecological equivalents to replace species deleted because of low population numbers. Two major refinements that changed the research thrust were (1) the inclusion of Aleut hunters and fishers on the biological expedition itself to ensure that subsistence foods and methods were represented, and (2) the addition of a fisheries biologist on a NOAA research trawler to allow sampling of commercial fishes. Although the original research design called for the collection of biota by Aleut subsistence fishermen, and by a commercial fishing boat, the research was modified with continued stakeholder input to actually include Aleuts and a fisheries biologist on the expeditions to ensure their representation. The inclusion of stakeholders during the development of protocols and the research itself improved the overall quality of the investigation, while making it more relevant to the interested and affected parties. Final responsibility for the design and execution of the research and radionuclide analysis rested with the researchers, but the process of stakeholder inclusion made the research more valuable as a source of credible information and for public policy decisions.     

Quantifying the transfer of radionuclides to food products from domestic farm animals

Databases have been compiled to derive parameter values relevant to the transfer of radionuclides from feedstuffs to domestic animal products to provide a revision to the IAEA Handbook on transfer parameters TRS 364. Significant new data inputs have been incorporated into the databases from an extensive review of Russian language information and inclusion of data published since the early 1990s. Fractional gastrointestinal absorption in adult ruminants presented in the revised handbook are generally similar to those recommended for adult humans by the ICRP. Transfer coefficient values are presented in the handbook for a range of radionuclides to farm animal products. For most animal products, transfer coefficient values for elements additional to those in TRS 364 are provided although many data gaps remain. Transfer coefficients generally vary between species with larger species having lower values than smaller species. It has been suggested that the difference is partly due to the inclusion of dietary dry matter intake in the estimation of transfer coefficient and that whilst dietary intake increases with size nutrient concentrations do not. An alternative approach to quantifying transfer by using concentration ratios (CR), which do not consider dietary intake, has been evaluated. CR values compiled for the handbook vary considerably less between species than transfer coefficient values. The advantage of the CR approach is that values derived for one species could be applied to species for which there are no data. However, transfer coefficients will continue to be used as few studies currently report CR values or give data from which they can be estimated.