RESUMEN
Tests using reconstituted samples have been performed to assess the diffusive transport of (137)Cs and (60)Co through natural regolith materials from a region in South Australia being considered for a radioactive waste repository. A double diffusion cell apparatus made of polycarbonate resin was developed to estimate the effective diffusion (D(e)) and sorption coefficients (K(d)) that allowed large withdrawals from the source and collector cells and has enabled tests with low concentrations of radioactivity. An alternative to porous stainless steel filter plates has also been used to reduce uncertainty in test interpretation. Analysis of the transient data used a staged method of the Laplace transform to take into consideration the volume of the samples withdrawn from the apparatus during testing. At test completion samples were cut into slices and analysed for radionuclide concentration. Data obtained from the sliced samples confirmed that both numerical and experimental data produced acceptable mass balance. The D(e) values obtained in this study were of the order of 10(-6) cm(2) s(-1) for both species, higher than previously published data. The K(d) values from the diffusion and batch sorption tests were in reasonable agreement for (137)Cs, but an order of magnitude different for (60)Co. The sorption of the latter radionuclide was strongly pH dependent, and this dependency during diffusion tests would benefit from further investigation.
Asunto(s)
Radioisótopos de Cesio/análisis , Radioisótopos de Cobalto/análisis , Monitoreo de Radiación , Contaminantes Radiactivos del Suelo/análisis , Radioisótopos de Cesio/química , Radioisótopos de Cobalto/química , Difusión , Conductividad Eléctrica , Concentración de Iones de Hidrógeno , Cinética , Contaminantes Radiactivos del Suelo/químicaRESUMEN
Arsenic is naturally associated with gold mineralisation and elevated in some soils and mine waste around historical gold mining activity in Victoria, Australia. To explore uptake, arsenic concentrations in children's toenail clippings and household soils were measured, and the microdistribution and speciation of arsenic in situ in toenail clipping thin sections investigated using synchrotron-based X-ray microprobe techniques. The ability to differentiate exogenous arsenic was explored by investigating surface contamination on cleaned clippings using depth profiling, and direct diffusion of arsenic into incubated clippings. Total arsenic concentrations ranged from 0.15 to 2.1 microg/g (n=29) in clipping samples and from 3.3 to 130 microg/g (n=22) in household soils, with significant correlation between transformed arsenic concentrations (Pearson's r=0.42, P=0.023) when household soil was treated as independent. In clipping thin sections (n=2), X-ray fluorescence (XRF) mapping showed discrete layering of arsenic consistent with nail structure, and irregular arsenic incorporation along the nail growth axis. Arsenic concentrations were heterogeneous at 10x10 microm microprobe spot locations investigated (<0.1 to 13.3 microg/g). X-ray absorption near-edge structure (XANES) spectra suggested the presence of two distinct arsenic species: a lower oxidation state species, possibly with mixed sulphur and methyl coordination (denoted As(approximately III)(-S, -CH3)); and a higher oxidation state species (denoted As(approximately V)(-O)). Depth profiling suggested that surface contamination was unlikely (n=4), and XRF and XANES analyses of thin sections of clippings incubated in dry or wet mine waste, or untreated, suggested direct diffusion of arsenic occurred under moist conditions. These findings suggest that arsenic in soil contributes to some systemic absorption associated with periodic exposures among children resident in areas of historic gold mining activity in Victoria, Australia. Future studies are required to ascertain if adverse health effects are associated with current levels of arsenic uptake.
Asunto(s)
Arsénico/metabolismo , Exposición a Riesgos Ambientales/análisis , Minería , Uñas/metabolismo , Contaminantes del Suelo/metabolismo , Dedos del Pie , Adolescente , Arsénico/análisis , Arsénico/química , Niño , Preescolar , Monitoreo del Ambiente , Femenino , Oro , Humanos , Masculino , Suelo/análisis , Contaminantes del Suelo/análisis , Contaminantes del Suelo/químicaRESUMEN
Soils from different climatic regions of Australia were studied to determine their adsorption of (137)Cs, and the effect of microbial sulfate reduction on this adsorption. The soils consisted of a surface and regolith samples from the site of a proposed low and intermediate level radioactive waste repository in arid South Australia, and two red earth loam soils from an experimental plot in the tropical Northern Territory. The process of bacterial sulfate reduction substantially decreased the adsorption of (137)Cs to the arid and tropical soils, although extended incubation resulted in greater adsorption to the regolith sample. This could have implications for the mobility of radionuclides entering these soil ecosystems.