Transfer of 129I to freshwater fish species within Fukushima and Chernobyl exclusion zones.

Unique data is reported on the transfer of 129I iodine from freshwaters to fish as well as the internal distribution within fish from the Fukushima and Chernobyl exclusion zones (ChEZ). Samples of water, sediments and fish were collected in the contaminated ponds Inkyozaka and Suzuuchi, and in the less contaminated Abukuma river in Fukushima, as well as in the contaminated Glubokoye lake and in the less contaminated Starukha lake in ChEZ. In water, 129I was mainly present as low molecular mass (LMM) and negatively charged species, while a minor fraction was associated with colloidal fraction, most probably organic material in water. The sediment-water 129I apparent distribution coefficients, Kd, ranged from 225 to 329 L/kg, equal that of stable iodine, but did not correlate with 129I/127I ratio or 129I/137Cs ratio as the environmental distribution of radioactive iodine was different from that of stable iodine and radioactive cesium. Concentration ratios (CR) of 129I in muscle of freshwater fish ranged from 85 to 544 across waterbodies with limited water exchange, similar in Fukushima and Chernobyl, but varied with respect to fish species. Thus, this is the first results on the transfer of 129I to freshwater fish, showing that the CR for freshwater fish is higher than CR reported for marine fish. Concentrations of 129I in fish muscle were, however, lower than in the intestinal content, indicating the influence of more contaminated dietary ingredients probably of terrestrial origin based due to δ13C signal on as well as of biodilution. The present results highlighted also that the radiation dose in fish was highly inhomogeneously distributed. Based on the present 129I/127I atomic ratio of 10-5 in the most contaminated fish in the ponds in Fukushima and Glubokoye lake in Chernobyl, however, a radiation dose of 10 µSv/y would not pose any harm to the fish population.

Natural radioactivity and element characterization in pit lakes in Northern Sweden.

Northern Sweden has been the object of intense metal mining in the last decades producing several water-filled open-pits, or pit lakes. Most of these pit lakes have been limed to maintain a good water quality and to prevent generation of acidic water that could leach the exposed rocks and release metals into water. The aim of this work was to examine the concentration of stable elements and naturally occurring radionuclides in water and sediment samples from pit lakes originating from non-uranium mining activities in Northern Sweden. Surface water and surface sediments were collected from 27 pit lakes in Northern Sweden. Water quality parameters, concentration of stable elements and radionuclides were measured by a water probe, ICP-MS and XRF, and alpha and gamma spectrometry, respectively. Furthermore, a multivariate statistical analysis (PCA) was performed on the water samples and sediments. In general, the quality of the surface water was good, but some lakes had low pH values (2.5-5.7), and high concentrations of Fe (up to 200 mg/L) and other metals (e.g. Zn, Cu). When relating the metal concentrations in sediments in pit lakes with the concentration found in natural lakes, some sites had relatively high levels of Cu, As, Cr and Pb. The activity concentration of 210Po, and U and Th isotopes in water and sediment samples were at environmental levels, as was the ambient dose equivalent rate at these sites (range 0.08-0.14 µSv/h).

The naturally occurring radioactivity of 'scalar energy' pendants and concomitant radiation risk.

Forming part of a study of radiological risk arising from use of radioactive consumer products, investigation is made of pendants containing naturally occurring radioactive material. Based on use of gamma-ray spectrometry and Monte Carlo (MC) simulations, the study investigates commercially available 'scalar energy pendants'. The doses from these have been simulated using MIRD5 mathematical phantoms, evaluation being made of dose conversion factors (DCFs) and organ dose. Metallic pendants code MP15 were found to contain the greatest activity, at 7043 ± 471 Bq from 232Th, while glass pendants code GP11 were presented the greatest 238U and 40K activity, at 1001 ± 172 and 687 ± 130 Bq respectively. MP15 pendants offered the greatest percentage concentrations of Th, Ce, U and Zr, with means of 25.6 ± 0.06, 5.6 ± 0.005, 1.03 ± 0.04 and 28.5 ± 0.08 respectively, giving rise to an effective dose of 2.8 mSv for a nominal wearing period of 2000 h. Accordingly, these products can give rise to annual doses in excess of the public limit of 1 mSv.

Environmental radioactivity and trace metals in surficial sediments from estuarine systems in Ghana (Equatorial Africa), impacted by artisanal gold-mining.

This paper reports concentrations of γ-emitter radionuclides (40K, 137Cs, 210Pb, 226Ra, 228Ra, 228Th and 234Th) and some metals (Al, Cr, Fe, Co, Ni, Cu, Zn, As, Sr, Cd, Sb, Cs, Pb, Th and U) in surficial sediments from the Ankobra, Pra and Volta estuaries, in Ghana. Artisanal gold-mining in the Ankobra and Pra basins promoted moderate enrichments of As, Sb, Cu, Cs and Cr in their estuarine sediments, with respect to the reference background of the Volta Estuary. Radionuclide concentrations were in the range found in the Earth's crust. Present data do not support any conclusion on their potential enrichments due to gold-mining activities. Radionuclide isotopic ratios revealed a transfer of 228Ra from sediments to the water column. Pearson correlation coefficient matrices showed different patterns, which were reasonably understood after novel approaches: i) inter-estuaries comparison of slopes in the linear regressions of element-concentrations vs Al, Fe and Cs; ii) study of Al-normalized concentrations of elements; iii) excess 210Pb informing on local sedimentary conditions. The metal enrichments observed in the Ankobra and Pra estuaries are associated with the Fe-rich compounds in sulphide ores (such as FeAsS) transported along the river course and deposited in the estuary.

Evaluation of the radioactive pollution in the salt-marshes under a phosphogypsum stack system.

Next to the city of Huelva (SW of Spain), around 100 Mt of phosphogypsum (PG) are stored in stacks on the salt-marshes of the Tinto River estuary covering a surface of about 1000 ha. Due to the high content of 238U series natural radionuclides of the PG, its acidic nature (pH about 3), and the fact that PG stacks were disposed without any kind of isolation from the substrate, they could produce a potential radioactive impact into the underlying sediments. The aim of this work is to assess the pollution of the underlying sediments by natural radionuclides coming from the PG stacks. To this end, seven cores were taken, and PG and sediments samples collected at different depths were analysed. The activity concentrations of the main long half-live natural radionuclides of interest were determined by applying both gamma-ray and alpha-particle spectrometry radiometric techniques. The results of this study showed that the first decimeters of salt-marsh sediment act as a "barrier" for the radionuclides coming from the PG stacks decreasing rapidly its activity concentration in depth, affecting mainly sediments located in the first 20 cm below the contact due to mixing processes. While 230Th, 226Ra and 210Pb pollution is mainly restricted to the first 20 cm of sediments, U-isotopes can reach higher depths (up to around 50 cm) by leaching processes due to their lower reactivity and higher concentration in the polluted leachates. The obtained results have high relevance for the design of the perimeter channel which is projected to build in the restoration project, suggesting that should has around 1 m deep under the base of the PG stacks, to ensure the full collection of polluting leachates, and to prevent their release into the estuary of the Tinto River.

Experimental study on the use of granulometric speciation for the radiometric dating of recent sediments.

Theoretical and experimental studies have shown that activity concentrations of fallout radionuclides (such as 137Cs and excess 210Pb) decrease with particles size in aqueous suspensions. This paper is aimed at reviewing the theoretical fundamentals for granulometric speciation of radionuclides, and at exploring its practical use in the analytical context of gamma spectrometry for the radiometric dating of recent sediments, with view to: i) improving the detection of 137Cs (since its use as independent chronostratigraphic mark is challenging in the southern hemisphere because its low fallout rate), ii) supporting refined CIC models and normalization techniques in 210Pb-based radiogeochronologies. The work uses surface sediments sampled from the Tinto Estuary (SW Spain), affected by mining and phosphate-fertilizer industries, and from the Ankobra Estuary (Ghana), affected by intensive artisanal gold-mining. Granulometric classes have been separated by a sieving column with decreasing mesh sizes and the obtained cumulative percentage of mass mathematically described by a Rosin-Rammler particle-size distribution. The target radionuclides for gamma spectrometry were 210Pb, 226Ra and137Cs, complemented with 40K, 234Th and 228Ra. Results revealed that, far from ideal experiments, under actual environmental conditions the increase in activity concentrations with decreasing particle sizes is too moderate, and in general they are affected by larger counting uncertainties due to the small available amount of mass. Indeed, there was no correlation between grain-size and 137Cs concentrations (p = 0.25), and similarly for excess 210Pb (p = 0.53). No effect of the organic matter content was observed in 137Cs (p = 0.58) and excess 210Pb (p = 0.85) concentrations. Present results pose some concerns to the general use of granulometric speciation in the context of gamma spectrometry for supporting the radiometric dating of recent sediments. A detailed discussion on the use of normalization methods is also presented.

Pollution evaluation on the salt-marshes under the phosphogypsum stacks of Huelva due to deep leachates.

In the salth-marshes of the Tinto River (Huelva estuary, SW Spain), are stored in stacks around 100 Mt of PG, covering a surface of 1000 ha without any type of isolation, which produce an important impact in the surrounding environment. On the other hand, this ecosystem it is affected by acid mine drainage (AMD) from sulphide mines located upstream the Tinto River. The aim of this study is to evaluate the deep pollution of the underlain salt-marsh sediments due to leachates from the PG stacks. For that purpose, 7 cores were collected from zones 2 and 3 of the stacks, and PG and salt-marsh sediments samples from different depths were analyzed. The physicochemical parameters, mineralogy, granulometry and the concentration of the main elements of interest were determined in the samples. Most analysed salt-marsh sediments are not affected by PG stacks pollution, because sediments act as a "barrier" for the leachates from the PG, concentrating the contaminants in the first decimetres (0.5 m) under PG-sediments contact, and the deep infiltration is very limited. The obtained results suggest that the perimeter channel which is projected to build in the restauration project, should has a depth of 1 m below the level of the PG stacks for assuring the complete collection of leachates from the stacks, and avoid their liberation into the Tinto River estuary.

Journal of Environmental Radioactivity special issue: II International Conference on Radioecological Concentration Processes. (50 years later).

An international conference on Radioecological Concentration Processes was held in Seville, Spain, 6-9 November 2016 at the Centro Nacional de Aceleradores. It was attended by 160 participants from 35 different countries. This was the 2nd conference on this item since 1966, 50 years ago. The conference covered aspects of radiological important radionuclides on terrestrial, marine and freshwater environments and has allowed obtaining a clear picture of the status of the Radioecology as a consolidated discipline in the 21st century.

Challenges associated with the behaviour of radioactive particles in the environment.

A series of different nuclear sources associated with the nuclear weapon and fuel cycles have contributed to the release of radioactive particles to the environment. Following nuclear weapon tests, safety tests, conventional destruction of weapons, reactor explosions and fires, a major fraction of released refractory radionuclides such as uranium (U) and plutonium (Pu) were present as entities ranging from sub microns to fragments. Furthermore, radioactive particles and colloids have been released from reprocessing facilities and civil reactors, from radioactive waste dumped at sea, and from NORM sites. Thus, whenever refractory radionuclides are released to the environment following nuclear events, radioactive particles should be expected. Results from many years of research have shown that particle characteristics such as elemental composition depend on the source, while characteristics such as particle size distribution, structure, and oxidation state influencing ecosystem transfer depend also on the release scenarios. When radioactive particles are deposited in the environment, weathering processes occur and associated radionuclides are subsequently mobilized, changing the apparent Kd. Thus, particles retained in soils or sediments are unevenly distributed, and dissolution of radionuclides from particles may be partial. For areas affected by particle contamination, the inventories can therefore be underestimated, and impact and risk assessments may suffer from unacceptable large uncertainties if radioactive particles are ignored. To integrate radioactive particles into environmental impact assessments, key challenges include the linking of particle characteristics to specific sources, to ecosystem transfer, and to uptake and retention in biological systems. To elucidate these issues, the EC-funded COMET and RATE projects and the IAEA Coordinated Research Program on particles have revisited selected contaminated sites and archive samples. This COMET position paper summarizes new knowledge on key sources that have contributed to particle releases, including particle characteristics based on advanced techniques, with emphasis on particle weathering processes as well as on heterogeneities in biological samples to evaluate potential uptake and retention of radioactive particles.

An integrated automatic system to evaluate U and Th dynamic lixiviation from solid matrices, and to extract/pre-concentrate leached analytes previous ICP-MS detection.

Leached fractions of U and Th from different environmental solid matrices were evaluated by an automatic system enabling the on-line lixiviation and extraction/pre-concentration of these two elements previous ICP-MS detection. UTEVA resin was used as selective extraction material. Ten leached fraction, using artificial rainwater (pH 5.4) as leaching agent, and a residual fraction were analyzed for each sample, allowing the study of behavior of U and Th in dynamic lixiviation conditions. Multivariate techniques have been employed for the efficient optimization of the independent variables that affect the lixiviation process. The system reached LODs of 0.1 and 0.7ngkg-1 of U and Th, respectively. The method was satisfactorily validated for three solid matrices, by the analysis of a soil reference material (IAEA-375), a certified sediment reference material (BCR- 320R) and a phosphogypsum reference material (MatControl CSN-CIEMAT 2008). Besides, environmental samples were analyzed, showing a similar behavior, i.e. the content of radionuclides decreases with the successive extractions. In all cases, the accumulative leached fraction of U and Th for different solid matrices studied (soil, sediment and phosphogypsum) were extremely low, up to 0.05% and 0.005% of U and Th, respectively. However, a great variability was observed in terms of mass concentration released, e.g. between 44 and 13,967ngUkg-1.

Natural radionuclides in plants, soils and sediments affected by U-rich coal mining activities in Brazil.

Mining activities can increase the mobility of metals by accelerating the dissolution and leaching of minerals from the rocks and tailing piles to the environment and, consequently, their availability for plants and subsequent transfer to the food chain. The weathering of minerals and the disposal of coal waste in tailing piles can accelerate the generation of acid mine drainage (AMD), which is responsible for the higher dissolution of metals in mining areas. In this context, the behavior of U, Th and K in soils and sediment, and the transfer factor (TF) of 238U, 234U and 210Po for soybean, wheat, pine and eucalyptus cultivated around a coal mine in southern Brazil was evaluated. Alpha and gamma spectrometry were used for the measurements of the activity concentration of the radioelements. 210Po was the radionuclide that is most accumulated in the plants, especially in the leaves. When comparing the plant species, pine showed the highest TF values for 234U (0.311 ± 0.420) for leaves, while eucalyptus showed the highest TF for 238U (0.344 ± 0.414) for leaves. In general, TF were higher for the leaves of soybean and wheat when compared to the grains, and grains of wheat showed higher TF for 210Po and 238U than grains of soybean. Deviations from the natural U isotopic ratio were recorded at all investigated areas, indicating possible industrial and mining sources of U for the vegetables. A safety assessment of transport routes and accumulation of radionuclides in soils with a potential for cultivation is important, mainly in tropical areas contaminated with solid waste and effluents from mines and industry.

226Ra dynamic lixiviation from phosphogypsum samples by an automatic flow-through system with integrated renewable solid-phase extraction.

The release of 226Ra from phosphogypsum (PG) was evaluated by developing a novel tool for fully automated 226Ra lixiviation from PG integrating extraction/pre-concentration using a renewable sorbent format. Eight leached fractions (30mL each one) and a residual fraction were analyzed allowing the evaluation of dynamic lixiviation of 226Ra. An automatic system allows this approach coupling a homemade cell with a 226Ra extraction/pre-concentration method, which is carried out combining two procedures: Ra adsorption on MnO2 and its posterior co-precipitation with BaSO4. Detection was carried out with a low-background proportional counter, obtaining a minimum detectable activity of 7Bqkg-1. Method was validated by analysis of a PG reference material (MatControl CSN-CIEMAT 2008), comparing the content found in fractions (sum of leached fractions + residual fraction) to the reference value. PG samples from Huelva (Spain) were studied. 226Ra average activity concentration of the sum of leached fractions with artificial rainwater at pH 5.4±0.2 was 105±3Bqkg-1d.w. representing a 226Ra lixiviation of 37%; while at pH 2.0±0.2, it was 168±3Bqkg-1 d.w., which represents a 50%. Also, static lixiviation, maintaining the same experimental conditions, was carried out indicating that, for both considered pH, the 226Ra release from PG is up to 50% higher in a dynamic leaching that in a static one, may have both environmental and reutilization implications.

Natural radionuclides in lichens, mosses and ferns in a thermal power plant and in an adjacent coal mine area in southern Brazil.

The radio-elements 234U, 235U, 238U, 230Th, 232Th and 210Po were characterized in lichens, mosses and ferns species sampled in an adjacent coal mine area at Figueira City, Paraná State, Brazil, due to their importance for the assessment of human exposure related to the natural radioactivity. The coal is geologically associated with a uranium deposit and has been used as a fossil fuel in a thermal power plant in the city. Samples were initially prepared at LABIDRO (Isotopes and Hydrochemistry Laboratory), UNESP, Rio Claro (SP), Brazil. Then, alpha-spectrometry after several radiochemical steps was used at the Applied Nuclear Physics Laboratories, University of Seville, Seville, Spain, for measuring the activity concentration of the radionuclides. It was 210Po the radionuclide that most bio-accumulates in the organisms, reaching the highest levels in mosses. The ferns species were less sensitive as bio-monitor than the mosses and lichens, considering polonium in relation to other radionuclides. Fruticose lichens exhibited lower polonium content than the foliose lichens sampled in the same site. Besides biological features, environmental characteristics also modify the radio-elements absorption by lichens and mosses like the type of vegetation covering these organisms, their substrate, the prevailing wind direction, elevation and climatic conditions. Only 210Po and 238U correlated in ferns and in soil and rock materials, being particulate emissions from the coal-fired power plant the most probable U-source in the region. Thus, the biomonitors used were able to detect atmospheric contamination by the radionuclides monitored.

Uranium in the surrounding of San Marcos-Sacramento River environment (Chihuahua, Mexico).

The main interest of this study is to assess whether uranium deposits located in the San Marcos outcrops (NW of Chihuahua City, Mexico) could be considered as a source of U-isotopes in its surrounding environment. Uranium activity concentrations were determined in biota, ground, and surface water by either alpha or liquid scintillation spectrometries. Major ions were analyzed by ICP-OES in surface water and its suspended matter. For determining uranium activity in biota, samples were divided in parts. The results have shown a possible lixiviation and infiltration of uranium from geological substrate into the ground and surface water, and consequently, a transfer to biota. Calculated annual effective doses by ingestion suggest that U-isotopes in biota could not negligibly contribute to the neighboring population dose. By all these considerations, it is concluded that in this zone there is natural enhancement of uranium in all environmental samples analyzed in the present work.

Journal of Environmental Radioactivity special issue: international topical conference on Po and radioactive Pb isotopes.

An international conference on polonium (Po) and radioactive isotopes was held in Seville Spain, 26-28 October 2009 at the Centro Nacional de Aceleradores. It was attended by 138 participants from 38 different countries. The sessions covered all aspects on Po and lead (Pb) such as radiochemistry, terrestrial and marine radioecology, kinetics, sedimentation rates, atmospheric tracers, NORM industries and dose assessment.

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.

The cumulative effect of three decades of phosphogypsum amendments in reclaimed marsh soils from SW Spain: (226)Ra, (238)U 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.

Sequential extraction of 226Ra in sediments from an estuary affected historically by anthropogenic inputs of natural radionuclides.

Riverbed sediments from an estuary historically affected by wastes discharged by several phosphate fertiliser plants and enriched in uranium-series radionuclides were operationally speciated using a Tessier-based method. In each selective fraction the (226)Ra content was determined by alpha-particle spectrometry after radiochemical isolation and electrodeposition onto stainless steel planchets. These studies were performed in (226)Ra-polluted estuarine sediments collected one year after anthropogenic discharges had ceased in order to obtain useful information about the operational forms in which this radionuclide remains associated with the sediments at this time. The results obtained revealed that one year after (226)Ra inputs had stopped, the radionuclide was associated mostly with the more refractory forms. Consequently, it is possible to foresee little potential remobilisation of (226)Ra contamination from sediments to the aqueous phase in the future under normal environmental conditions.

Phosphogypsum amendment effect on radionuclide content in drainage water and marsh soils from southwestern Spain.

Phosphogypsum (PG) is a residue of the phosphate fertilizer industry that has relatively high concentrations of 226Ra and other radionuclides. Thus, it is interesting to study the effect of PG applied as a Ca amendment on the levels and behavior of radionuclides in agricultural soils. A study involving treatments with 13 and 26 Mg ha(-1) of PG and 30 Mg ha(-1) of manure was performed, measuring 226Ra and U isotopes in drainage water, soil, and plant samples. The PG used in the treatment had 510 +/- 40 Bq kg(-1) of 226Ra. The 226Ra concentrations in drainage waters from PG-amended plots were similar (between 2.6 and 7.2 mBq L(-1)) to that reported for noncontaminated waters. Although no significant effect due to PG was observed, the U concentrations in drainage waters (200 mBq L(-1) for 238U) were one order of magnitude higher than those described in noncontaminated waters. This high content in U can be ascribed to desorption processes mainly related to the natural adsorbed pool in soil (25 Bq kg(-1) of 238U). This is supported by the 234U to 238U isotopic ratio of 1.16 in drainage waters versus secular equilibrium in PG and P fertilizers. The progressive enrichment in 226Ra concentration in soils due to PG treatment cannot be concluded from our present data. This PG treatment does not determine any significant difference in 226Ra concentration in drainage waters or in plant material [cotton (Gossipium hirsutum L.) leaves]. No significant levels of radionuclides except 40K were found in the vegetal tissues.

Radioactive impact in sediments from an estuarine system affected by industrial wastes releases.

A big fertilizer industrial complex and a vast extension of phosphogypsum piles (12 km2), sited in the estuary formed by the Odiel and Tinto river mouths (southwest of Spain), are producing an unambiguous radioactive impact in their surrounding aquatic environment through radionuclides from the U-series. The levels and distribution of radionuclides in sediments from this estuarine system have been determined. The analyses of radionuclide concentrations and activity ratios have provided us with an interesting information to evaluate the extension, degree and routes of the radioactive impact, as well as for the knowledge of the different pathways followed for the radioactive contamination to disturb this natural system. The obtained results indicate that the main pathway of radioactive contamination of the estuary is through the dissolution in its waters of the radionuclides released by the industrial activities and their later fixation on the particulate materials. Tidal activity also plays an important role in the transport and homogenization along the estuary of the radioactivity released from the fertilizer plants.