The coastline near Chañaral in Northern Chile is one of the most highly Cu-contaminated zones in the world due to discharges from mining activities for more than 60 years. The speciation of Cu has been studied to determine the importance of organic complexation in highly contaminated areas, and to assess the likely physiological impacts of Cu on marine organisms. Dissolved Cu concentrations of up to 500 nM were measured, completely saturating organic ligands and leading to free Cu2+ concentrations in excess of 10− 8 M. These values are higher than those reported in any other marine environment, and because they occur over an extensive area, provide a unique opportunity to study the effects of Cu on marine ecosystems and to see how Cu behaves when its speciation is predominantly inorganic. We found strong gradients in free Cu2+ between Chañaral and adjacent areas with lower Cu, where speciation is dominated by organic complexation. There is also a significant increase in the partitioning of Cu onto suspended particles in the contaminated areas, consistent with previous studies that showed that organic ligands stabilize Cu in the dissolved phase, whilst “excess” Cu is rapidly scavenged. Those high dissolved Cu concentrations persist in spite of solid phase partitioning and advective processes along this open-ocean coastline, suggesting that Cu inputs into the system are still very large. Measurements were made using anodic stripping voltammetry with a thin mercury film coated with Nafion, which previous workers have shown can mitigate ambiguity in the data arising from inadvertent reduction of organic complexes. Our findings suggest that this is a useful methodology for contaminated systems. 相似文献
This paper presents the results of investigation on uptake of radioactive species 90Sr and 137Cs present in the liquid effluents from nuclear processing plants. Chemical precipitation process is adopted to remove radioactivity from the effluents with low and intermediate level of activity. In this process, radioactive 90Sr and 137Cs are co-precipitated along with copper ferrocyanide, ferric hydroxide and either calcium phosphate or barium sulphate. These precipitates being fine in size require flocculation for enhanced settling rate in clarifier/thickener. The flocculation by some selected high molecular weight polyacrylamide based polymers has improved the uptake of radioactive metal ions. The adsorption of these radioactive species has been found to increase in the presence of these flocculants thereby improving the decontamination factor (DF). While flocculating the precipitates, there may be some complex formation with Sr2+/Cs+, flocculant and the substrate. This has enhanced the uptake of the radioactive metal ions from the liquid component. The plant trials have indicated the improvement of DF value due to flocculation by cationic flocculant. 相似文献
The Irtysh river basin all the way from river spring in China across Kazakhstan as far as the Russian part of Siberia is among the most ecologically endangered and affected regions on our planet. The study provides a summary of the historical reasons for anthropological interventions in this area, which began with the construction of plants of the military—industrial complexes in the forties of the last century during World War II. These plants have a major share in extreme high concentrations of heavy metals in surface as well in groundwaters locally. The Semipalatinsk nuclear polygon plays a specific role as a source of contamination of local waters. The release of top secret data enabled us to gain knowledge about serious problems related to high radioactivity of groundwaters, which should spread uncontrollably through a system of secondary fissures activated by nuclear blasts. Another serious problem in this region is the quantitative aspect of contamination. Model simulations of water balance indicate that large industrial development in the spring area in China and continuously increasing water consumption in Kazakhstan may lead to desiccation of the lower stretch of this large river in Siberia during the summer months of 2030. 相似文献
Natural production of the radionuclide chlorine-36 (36Cl) has provided a valuable tracer for groundwater studies. The nuclear industry, especially the testing of thermonuclear
weapons, has also produced large amounts of 36Cl that can be detected in many samples of groundwater. In order to be most useful in hydrologic studies, the natural production
prior to 1952 should be distinguished from more recent artificial sources. The object of this study was to reconstruct the
probable preanthropogenic levels of 36Cl in groundwater in the United States. Although significant local variations exist, they are superimposed on a broad regional
pattern of 36Cl/Cl ratios in the United States. Owing to the influence of atmospherically transported ocean salt, natural ratios of 36Cl/total Cl are lowest near the coast and increase to a maximum in the central Rocky Mountains of the United States.
Electronic Publication 相似文献
The understanding of the thermo-hydro-mechanical behaviour of a clay barrier is needed for the prediction of its final in situ properties after the hydration and thermal transient in a radioactive waste repository.
As part of the CEC 1990–1994 R&D programme on radioactive waste management and storage, the CEA (Fr), CIEMAT (Sp), ENRESA (Sp), SCK · CEN (B), UPC (Sp) and UWCC (UK) have carried out a joint project on unsaturated clay behaviour (Volckaert et al., 1996). The aim of the study is to analyse and model the behaviour of a clay-based engineered barrier during its hydration phase under real repository conditions. The hydro-mechanical and thermo-hydraulic models developed in this project have been coupled to describe stress/strain behaviour, moisture migration and heat transfer. A thermo-hydraulic model has also been coupled to a geochemical code to describe the migration and formation of chemical species.
In this project, suction-controlled experiments have been performed on Boom clay (B), FoCa clay (Fr) and Almeria bentonite (Sp). The aim of these experiments is to test the validity of the interpretive model developed by Alonso and Gens (Alonso et al., 1990), and to build a database of unsaturated clay thermo-hydro-mechanical parameters. Such a database can then be used for validation exercises in which in situ experiments are simulated.
The Boom clay is a moderately swelling clay of Rupellian age. It is studied at the SCK · CEN in Belgium as a potential host rock for a radioactive waste repository. In this paper, suction-controlled experiments carried out on Boom clay by SCK · CEN are described. SCK · CEN has performed experiments to measure the relation between suction, water content and temperature and the relation between suction, stress and deformation. The applied suction-control techniques and experimental setups are detailed. The results of these experiments are discussed in the perspective of the model of Alonso and Gens. The influence of temperature on water uptake was rather small. The measured swelling-collapse behaviour can be explained by the Alonso and Gens model. 相似文献
Tooeleite, nominally Fe63+(As3+O3)4(SO4)(OH)4·4H2O, is a relatively uncommon mineral of some acid-mine drainage systems. Yet, if it does occur, it does so in large quantities, indicating that some specific conditions favor the formation of this mineral in the system Fe-As-S-O-H. In this contribution, we report the thermodynamic properties of synthetic tooeleite. The sample was characterized by powder X-ray diffraction, scanning electron microscopy, extended X-ray absorption fine-structure spectroscopy, and Mössbauer spectroscopy. These methods confirmed that the sample is pure, devoid of amorphous impurities of iron oxides, and that the oxidation state of arsenic is 3+. Using acid-solution calorimetry, the enthalpy of formation of this mineral from the elements at the standard conditions was determined as −6196.6 ± 8.6 kJ mol−1. The entropy of tooeleite, calculated from low-temperature heat capacity data measured by relaxation calorimetry, is 899.0 ± 10.8 J mol−1 K−1. The calculated standard Gibbs free energy of formation is −5396.3 ± 9.3 kJ mol−1. The log Ksp value, calculated for the reaction Fe6(AsO3)4(SO4)(OH)4·4H2O + 16H+ = 6Fe3+ + 4H3AsO3 + SO42− + 8H2O, is −17.25 ± 1.80. Tooeleite has stability field only at very high activities of aqueous sulfate and arsenate. As such, it does not appear to be a good candidate for arsenic immobilization at polluted sites. An inspection of speciation diagrams shows that the predominance field of Fe3+ and As3+ overlap only at strongly basic conditions. The formation of tooeleite, therefore, requires strictly selective oxidation of Fe2+ to Fe3+ and, at the same time, firm conservation of the trivalent oxidation state of arsenic. Such conditions can be realized only by biological systems (microorganisms) which can selectively oxidize one redox-active element but leave the other ones untouched. Hence, tooeleite is the first example of an “obligatory” biomineral under the conditions prevailing at or near the Earth's surface because its formation under these conditions necessitates the action of microorganisms. 相似文献
Sodalites have been proposed as a possible host of certain radioactive species, specifically 99Tc and 129I, which may be encapsulated into the cage structure of the mineral. To demonstrate the ability of this framework silicate mineral to encapsulate and immobilize 99Tc and 129I, single-pass flow-through (SPFT) tests were conducted on a sodalite-bearing multi-phase ceramic waste form produced through a steam reforming process. Two samples made using a steam reformer samples were produced using non-radioactive I and Re (as a surrogate for Tc), while a third sample was produced using actual radioactive tank waste containing Tc and added Re. One of the non-radioactive samples was produced with an engineering-scale steam reformer while the other non-radioactive sample and the radioactive sample were produced using a bench-scale steam reformer. For all three steam reformer products, the similar steady-state dilute-solution release rates for Re, I, and Tc at pH (25 °C) = 9 and 40 °C were measured. However, it was found that the Re, I, and Tc releases were equal or up to 4.5x higher compared to the release rates of the network-forming elements, Na, Al, and Si. The similar releases of Re and Tc in the SPFT test, and the similar time-dependent shapes of the release curves for samples containing I, suggest that Re, Tc, and I partition to the sodalite minerals during the steam reforming process. 相似文献