J.M. Abril

Some physical and chemical features of the variability of kd distribution coefficients for radionuclides

kd distribution coefficients are widely used as a first approach to the understanding and determination of the eventual fate of metals and radionuclides released into the aquatic environment. For some radionuclides, kd varies within a range of more than two orders of magnitude. Based on some physical and chemical aspects of the interactions between the dissolved and the particulate phases, some mathematical equations have been developed to explain some features of the observed kd variability quantitatively. Thus, we have studied the decrease in particle size of kd in the case of man-made radionuclides interacting with natural particles, and its increase in the case of naturally occurring radionuclides. For the latter, the dependence of kd on the instantaneous water state has also been investigated. The study also shows the competition effects, particularly the dependence of kd on pH and salinity. Finally, the effects produced by the size distribution of a given population of particles or the mixture of different populations, are also included. The present work provides for each situation, experimental support from literature data and/or modelling exercises.

Modelling the dispersion of non-conservative radionuclides in tidal waters—Part 1: Conceptual and mathematical model

Abstract A 2D four-phase model to study the dispersion of non-conservative radionuclides in tidal waters, in conditions of disequilibrium for ionic exchanges, has been developed. At disequilibrium conditions, ionic exchanges cannot be formulated using distribution coefficients k d . Thus, kinetic transfer coefficients have been used. The model includes ionic exchanges among water and the solid phases (suspended matter and two grain size fractions of sediments), the deposition and resuspension of suspended matter and advective plus diffusive transport. In the second part of this work, which is presented in a separate paper, the model is applied to simulate 226 Ra dispersion, discharged from a fertilizer processing plant, in an estuarine system in the south-west of Spain.

The cumulative effect of three decades of phosphogypsum amendments in reclaimed marsh soils from SW Spain : 226Ra, 238U and Cd contents in soils and tomato fruit

Phosphogypsum (PG), a by-product of the phosphate fertiliser industries, has been applied as soil amendment to reduce Na saturation in soils, as in the reclaimed marsh area from SW Spain, where available PG has a typical fingerprint of 710+/-40 Bq kg(-1) of (226)Ra, 165+/-15 Bq kg(-1) of (238)U and 2.8+/-0.4 mg kg(-1) of Cd. This work was focussed on the cumulative effects of PG amendments on the enrichment of these pollutants in cultivated soils and plants (Lycopersicum esculentum Mill L.) from the area studied, where PG has been applied since 1978 at recommended rates of 20-25 Mg ha(-1) every 2-3 years. A field experiment was conducted over three years to compare activity concentrations of (226)Ra ((214)Pb) and (238)U ((234)Th) in non-reclaimed soils, reclaimed soils with no additional PG application, and reclaimed soils with two additional PG applications. A non-significant effect of two PG amendments (in three years) was observed when compared with non-amended reclaimed plots. Nevertheless, a significant (p<0.05) enrichment of (226)Ra was observed in the surface horizon (0-30 cm) of reclaimed plots relative to deeper horizons and also when compared with the surface horizon of non-reclaimed soil (p<0.05), thereby revealing the cumulative effect of three decades of PG applications. Furthermore, the effect of a continuous application of PG was studied by analysing soils and tomato fruits from six commercial farms with different cumulative rates of PG applied. Cadmium concentrations in tomatoes, which were one order of magnitude higher than those found in tomatoes from other areas in South Spain, were positively correlated (r = 0.917) with (226)Ra-concentration in soils, which can be considered an accurate index of the cumulative PG rate of each farm.

Modelling the suspended matter distribution in an estuarine system. Application to the Odiel river in southwest Spain

Abstract A numerical model which solves the advective-diffusive dispersion equation for suspended matter and includes the deposition and resuspension is presented. The model requires the simultaneous solution of the hydrodynamic equations under tidal dynamics and atmospheric forcing, using time steps of a few seconds. The model has been applied to the Odiel river (southwest Spain). The hydrodynamic module has been widely validated for neap and medium tides, whereas the dispersion was calibrated against the dissolved 226Ra dispersion pattern. This 226Ra is discharged to the Odiel river from a phosphate fertilizer factory. The model was able to reproduce the observed behaviour of the suspended matter in the estuary. The sedimentation rates have shown that a net, although slow, sedimentation is being produced. Sensitivity tests were inconclusive with respect to parameters describing settling and resuspension, as internal processes within the estuary are overridden by the high influx and efflux of particulate material from the sea.

Dating of marine sediments by an incomplete mixing model

Abstract A marine sediment core from the Kattegat area (Sweden) has been studied for dating purposes. The 137 Cs and 210 Pb profiles have been measured and described by a model of incomplete activity mixing. A time-dependent 137 Cs flux function for the sediment has been constructed from atmospheric data and the 137 Cs contents in water from the Sellafield nuclear reprocessing plant. It has been used as the 137 Cs input function for our model. The results show that the model clearly reproduces the measured profile.

Experimental and modelling study of plutonium uptake by suspended matter in aquatic environments from southern Spain.

Kinetic transfer coefficients are important parameters to understand and reliably model the behaviour of non-conservative radionuclides in aquatic environments. This report pertains to a series of five radiotracer experiments on Pu uptake in natural aqueous suspensions of unfiltered waters from three aquatic systems in the south of Spain (Gergal reservoir, the Guadalquivir river, and the estuary of the Tinto river). The experimental procedure ensured the simulation of environmental conditions. Pu activity was measured by a liquid scintillation technique. The uptake curves, covering a period up to one week, are discussed with respect to numerical uptake kinetics models. The data suggest that in our experimental setting the main pathways for Pu uptake consist of two parallel and reversible reactions followed by a consecutive non-reversible reaction. Kinetic transfer coefficients were estimated by a fitting procedure and a comparative study was followed.

Extensive radioactive characterization of a phosphogypsum stack in SW Spain: 226Ra, 238U, 210Po concentrations and 222Rn exhalation rate.

Phosphogypsum (PG) is a by-product of the phosphate fertilizer industries that contains relatively high concentrations of uranium series radionuclides. The US-EPA regulates the agriculture use of PG, attending to its (226)Ra content and to the (222)Rn exhalation rate from inactive stacks. Measurements of (222)Rn exhalation rates in PG stacks typically show a large and still poorly understood spatial and temporal variability, and the published data are scarce. This work studies an inactive PG stack in SW Spain of about 0.5 km(2) from where PG can be extracted for agriculture uses, and an agriculture soil 75 km apart, being representative of the farms to be amended with PG. Activity concentrations of (226)Ra, (238)U and (210)Po have been measured in 30 PG samples (0-90 cm horizon) allowing for the construction of maps with spatial distributions in the PG stack and for the characterization of the associated PG inputs to agriculture soils. Averaged (226)Ra concentrations for the stack were 730+/-60 Bq kg(-1) (d.w.), over the US-EPA limit of 370 Bq kg(-1). (222)Rn exhalation rate has been measured by the charcoal canister method in 49 sampling points with 3 canisters per sampling point. Values in PG stack were under the US-EPA limit of 2600 Bq m(-2)h(-1), but they were one order of magnitude higher than those found in the agriculture soil. Variability in radon emissions has been studied at different spatial scales. Radon exhalation rates were correlated with (226)Ra concentrations and daily potential evapotranspiration (ETo). They increased with ETo in agriculture soils, but showed an opposite behaviour in the PG stack.

Kinetic transfer coefficients for radionuclides in estuarine waters: Reference values from133Ba and effects of salinity and suspended load concentration

In estuarine environments there are important spatial and temporal changes in both salt and suspended load concentrations. An experimental procedure have been developed to produce kinetic parameters being representative of the natural environment studied, and we have investigated the effect of salinity and suspended load concentration to the kinetics of the uptake. These results are encouraged by recent advances in environmental modelling concerning to radionuclide dispersion in aquatic natural systems and involving non-equilibrium processes. Experiments are carried out with unfiltered water samples from the Odiel estuary (Southwest of Spain), with133Ba tracer to illustrate experimental procedures.

Modelling the dispersion of non-conservative radionuclides in tidal waters—Part 2: Application to 226Ra dispersion in an estuarine system

Abstract The Odiel river is an estuary system located in the south-west of Spain and affected by tidal dynamics. A phosphate fertilizer processing plant releases part of its wastes directly into the Odiel river. The model described in a previous paper ( J. Environ. Radioactivity , 31 (2), 127–141 ) has been applied to study 226 Ra (discharged from the fertilizer plant) dispersion in the Odiel river. The model adequately reproduces the observed behaviour of 226 Ra in suspended matter and the dissolved phase along the Odiel river, as well as the general behaviour of the measured distribution coefficients. Some predictive studies as well as the corresponding sensitivity studies are also included in this paper.

A 2D 4-phases marine dispersion model for non-conservative radionuclides. Part 1: Conceptual and computational model

Abstract Modelling the dispersion of non-conservative radionuclides in a given marine environment involves a wide set of complex processes: horizontal water movements (advection and diffusion), suspended matter dynamics, sediment composition, accumulation or erosion rates, continental water input and its dispersion pattern, evaporation-precipitation balance and the ionic exchange among the different phases. In this paper we present the conceptual and computational basis of a mathematical model which includes all the above processes. This model has been developed in different stages, in such a way that every new step includes the previously validated model and is subject to a further validation. Here, the sub-grid scale processes, such as the ionic exchanges and other activity transfers among phases, are included. In the second part of this work, which is presented in a separate paper, the model is applied and validated using studies of 137Cs and 239 + 240Pu dispersion in the Irish Sea.