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.     

Probabilistic distribution coefficients (Kds) in freshwater for radioisotopes of Ag,Am, Ba,Be, Ce,Co, Cs,I, Mn,Pu, Ra,Ru, Sb,Sr and Th – implications for uncertainty analysis of models simulating the transport of radionuclides in rivers

The objective of this study was to provide operational probability density functions (PDFs) for distribution coefficients (K_ds) in freshwater, representing the partition of radionuclides between the particulate and the dissolved phases respectively. Accordingly, the K_d variability should be considered in uncertainty analysis of transport and risk assessment models. The construction of PDFs for 8 elements (Ag, Am, Co, Cs, I, Mn, Pu and Sr) was established according to the procedure already tested in Durrieu et al. [2006. A weighted bootstrap method for the determination of probability density functions of freshwater distribution coefficients (K_ds) of Co, Cs, Sr and I radioisotopes. Chemosphere 65 (8), 1308–1320]: (i) construction of a comprehensive database where K_ds values obtained under various environments and parametric conditions were collected; (ii) scoring procedure to account for the ‘quality’ of each datapoint (according to several criteria such as the presentation of data (e.g. raw data vs mean with or without replicates), contact time, pH, solid-to-liquid ratio, expert judgement) in the construction of the PDF; (iii) weighted bootstrapping procedure to build the PDFs, in order to give more importance to the most relevant datapoints. Two types of PDFs were constructed: (i) non-conditional, usable when no knowledge about the site of concern is available; (ii) conditional PDFs corresponding to a limited range of parameters such as pH or contact time; conditional PDFs can thus be used when some parametric information is known on the site under study. For 7 other radionuclides (Ba, Be, Ce, Ra, Ru, Sb and Th), a simplified procedure was adopted because of the scarcity of data: only non-conditional PDFs were built, without incorporating a scoring procedure.     

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.     

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.     

化工污泥中放射性核素226Ra，232Th 的辐射环境行为

目的以化工生产下游企业排放含重金属污泥中放射性核素的分布与含量为研究对象,考察工业生产末端随物料流下行的重金属及其中携带的放射性核素对环境的影响。方法在重金属排放较为显著的电池、电镀化工企业采集含重金属污泥进行分析研究。利用高纯锗(HPGe)γ能谱仪系统分析不同类别污泥中放射性核素~(228)Ac,~(~(212))Pb,~(~(212))Bi,~(208)Tl,~(214)Pb,~(214)Bi和40K的活度和含量,选用蒙特卡罗模型(Monte Carlo N Particle Transport Code)剂量转化因子计算化工企业污泥的年有效剂量率,通过计算富集因子得到放射性核素~(232)Th,~(~(226))Ra在化工污泥中的富集水平,通过皮尔森系数将测量得到污泥中Pb,Cr等重金属含量以及相应的~(232)Th含量或镭当量活度Ra_(eq)相互关联,分析其中的数学相关性。结果来自电池、电镀化工企业的污泥中放射性有效剂量率为44.8μSv·a~(-1)。放射性核素~(232)Th,~(~(226))Ra的富集因子(EF-Th和EF-Ra)数值范围分别为0.478~2.217和2.509~4.115,表明放射性核素~(232)Th在含铬污泥中存在富集,而~(~(226))Ra在污泥中均存在明显富集。皮尔森系数的分析显示,重金属元素Pb和Cr与Ra_(eq)的相关性可达到0.8以上,在监测工作中可利用污泥中Pb,Cr含量推算含重金属污泥的放射性水平。结论该研究工作对辐射环境的快捷监测和TENORM的评价均有实际应用价值。     

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.     

Radiological impacts of phosphogypsum

This study was carried out to assess the radiological impact of Syrian phosphogypsum (PG) piles in the compartments of the surrounding ecosystem. Estimating the distribution of naturally occurring radionuclides (i.e. (226)Ra, (238)U, (232)Th, (210)Po and (210)Pb) in the raw materials, product and by-product of the Syrian phosphate fertilizer industry was essential. The data revealed that the concentrations of the radionuclides were enhanced in the treated phosphate ore. In PG, (226)Ra content had a mean activity of 318 Bq kg(-1). The uranium content in PG was low, ca. 33 Bq kg(-1), because uranium remained in the phosphoric acid produced. Over 80% of (232)Th, (210)Po and (210)Pb present partitioned in PG. The presence of PG piles did not increase significantly the concentration of (222)Rn or gamma rays exposure dose in the area studied. The annual effective dose was only 0.082 mSv y(-1). The geometric mean of total suspended air particulates (TSP) ca. 85 μg m(-3). The activity concentration of the radionuclides in filtrates and runoff waters were below the detection limits (ca. 0.15 mBq L(-1) for (238)U, 0.1 mBq L(-1) for (232)Th and 0.18 mBq L(-1) for both of (210)Po and (210)Pb); the concentration of the radionuclides in ground water samples and Qattina Lake were less than the permissible limits set for drinking water by the World Health Organisation, WHO, (10, 1 and 0.1 Bq L(-1) for (238)U, (232)Th and both of (210)Po and (210)Pb, respectively). Eastern sites soil samples of PG piles recorded the highest activity concentrations, i.e. 26, 33, 28, 61 and 40 Bq kg(-1) for (226)Ra, (238)U, (232)Th, (210)Po and (210)Pb, respectively, due to the prevailing western and north-western wind in the area, but remained within the natural levels reported in Syrian soil (13-32 Bq kg(-1) for (226)Ra, 24.9-62.2 Bq kg(-1) for (238)U and 10-32 Bq kg(-1) for (232)Th). The impact of PG piles on plants varied upon the plant species. Higher concentrations of the radionuclides were recorded for grass in comparison to broad-leaved plants. Among the species that grow naturally on PG piles, Inula, Ecballium and Polygonium may be radionuclides accumulators. A determined effort is needed at a national level to achieve a common and coherent approach to regulate PG piles or to consider it a resource material rather than waste or residue.     

Foliar and root uptake of Cs, Sr and Zn in processing tomato plants (Lycopersicon esculentum Mill.)

The results of an experimental study on the behaviour of ¹³⁴Cs, ⁸⁵Sr and ⁶⁵Zn in processing tomato plants grown in peat substrate are presented. Plants were contaminated by wet deposition of ¹³⁴Cs, ⁸⁵Sr and ⁶⁵Zn, either by sprinkling the above ground part at two phenological stages or by administering ¹³⁴Cs, ⁸⁵Sr and ⁶⁵Zn to the soil. The plants contaminated at the second phenological stage intercepted 38.3% less than those contaminated at the first stage, although leaf area increased by more than double. Transfer coefficients from peat soil to ripe fruit for ¹³⁴Cs are significantly higher than those for ⁸⁵Sr and ⁶⁵Zn. Leaf to fruit transfer coefficients for ¹³⁴Cs are one order of magnitude higher than for ⁶⁵Zn and two orders higher than for ⁸⁵Sr. Only when deposition affects fruits, as at the second phenological stage, are transfer coefficients to fruits similar for the three radionuclides.