Núria Casacuberta

Radioactivity contents in dicalcium phosphate and the potential radiological risk to human populations

Potentially harmful phosphate-based products derived from the wet acid digestion of phosphate rock represent one of the most serious problems facing the phosphate industry. This is particularly true for dicalcium phosphate (DCP), a food additive produced from either sulphuric acid or hydrochloric acid digestion of raw rock material. This study determined the natural occurring radionuclide concentrations of 12 DCP samples and 4 tricalcium phosphate (TCP) samples used for animal and human consumption, respectively. Metal concentrations (Al, Fe, Zn, Cd, Cr, As, Hg, Pb and Mg) were also determined. Samples were grouped into three different clusters (A, B, C) based on their radionuclide content. Whereas group A is characterized by high activities of 238U, 234U (approximately 10(3) Bq kg(-1)), 210Pb (2 x 10(3) Bq kg(-1)) and (210)Po ( approximately 800 Bq kg(-1)); group B presents high activities of (238)U, (234)U and (230)Th (approximately 10(3) Bq kg(-1)). Group C was characterized by very low activities of all radionuclides (< 50 Bq kg(-1)). Differences between the two groups of DCP samples for animal consumption (groups A and B) were related to the wet acid digestion method used, with group A samples produced from hydrochloric acid digestion, and group B samples produced using sulphuric acid. Group C includes more purified samples required for human consumption. High radionuclide concentrations in some DCP samples (reaching 2 x 10(3) and 10(3) Bq kg(-1) of 210Pb and 210Po, respectively) may be of concern due to direct or indirect radiological exposure via ingestion. Our experimental results based on 210Pb and 210Po within poultry consumed by humans, suggest that the maximum radiological doses are 11 +/- 2 microSv y(-1). While these results suggest that human health risks are small, additional testing should be conducted.

Reassessment of 90Sr, 137Cs, and 134Cs in the Coast off Japan Derived from the Fukushima Dai-ichi Nuclear Accident

The years following the Fukushima Dai-ichi nuclear power plant (FDNPP) accident, the distribution of (90)Sr in seawater in the coast off Japan has received limited attention. However, (90)Sr is a major contaminant in waters accumulated within the nuclear facility and in the storage tanks. Seawater samples collected off the FDNPP in September 2013 showed radioactive levels significantly higher than pre-Fukushima levels within 6 km off the FDNPP. These samples, with up to 8.9 ± 0.4 Bq·m(-3) for (90)Sr, 124 ± 3 Bq·m(-3) for (137)Cs, and 54 ± 1 Bq·m(-3) for (134)Cs, appear to be influenced by ongoing releases from the FDNPP, with a characteristic (137)Cs/(90)Sr activity ratio of 3.5 ± 0.2. Beach surface water and groundwater collected in Sendai Bay had (137)Cs concentrations of up to 43 ± 1 Bq·m(-3), while (90)Sr was close to pre-Fukushima levels (1-2 Bq·m(-3)). These samples appear to be influenced by freshwater inputs carrying a (137)Cs/(90)Sr activity ratio closer to that of the FDNPP fallout deposited on land in the spring of 2011. Ongoing inputs of (90)Sr from FDNPP releases would be on the order of 2.3-8.5 GBq·d(-1) in September 2013, likely exceeding river inputs by 2-3 orders of magnitude. These results strongly suggest that a continuous surveillance of artificial radionuclides in the Pacific Ocean is still required.

Determination of U and Th α-emitters in NORM samples through extraction chromatography by using new and recycled UTEVA resins.

This manuscript describes a protocol for the determination of U and Th isotopes via alpha spectrometry in NORM samples containing high concentrations of these radionuclides, up to kBq kg(-1). This technique is based on extraction chromatography with UTEVA (Triskem Int.) resins and it has been tested using both NORM samples from a phosphate industry and reference materials. The results proved that this method is highly optimized in terms of accuracy and precision when dealing with NORM samples. Recycling of UTEVA columns was also checked using NORM samples and successful results were obtained for both U and Th isotopes, thus proving the feasibility of re-using these type of columns.

Numerical Modeling of the Releases of 90Sr from Fukushima to the Ocean: An Evaluation of the Source Term

A numerical model consisting of a 3D advection/diffusion equation, including uptake/release reactions between water and sediments described in a dynamic way, has been applied to simulate the marine releases of (90)Sr from the Fukushima power plant after the March 2011 tsunami. This is a relevant issue since (90)Sr releases are still occurring. The model used here had been successfully applied to simulate (137)Cs releases. Assuming that the temporal trend of (90)Sr releases was the same as for (137)Cs during the four months after the accident simulated here, the source term could be evaluated, resulting in a total release of 80 TBq of (90)Sr until the end of June, which is in the lower range of previous estimates. Computed vertical profiles of (90)Sr in the water column have been compared with measured ones. The (90)Sr inventories within the model domain have also been calculated for the water column and for bed sediments. Maximum dissolved inventory (obtained for April 10th, 2011) within the model domain results in about 58 TBq. Inventories in bed sediments are 3 orders of magnitude lower than in the water column due to the low reactivity of this radionuclide. (90)Sr/(137)Cs ratios in the ocean have also been calculated and compared with measured values, showing both spatial and temporal variations.

Reconstruction of the 236U input function for the Northeast Atlantic Ocean: Implications for 129I/236U and 236U/238U‐based tracer ages

A reconstruction of historical discharges of 236U into the Northeast Atlantic Ocean by nuclear installations is presented. The nuclear reprocessing facilities Sellafield (SF), Great Britain (GB) and La Hague (LH), France and potentially also the nuclear fuel processing installation Springfields (SP), GB represent the main contributors of 236U in the Northeast Atlantic Ocean. Because data on 236U releases is lacking, 236U discharges from SP and SF are estimated based on the U-isotopic systematics found in the discharges from LH. The resulting reconstruction of 236U releases indicates that, until 2013, a total of (95±32) kg of 236U was discharged from SF, SP, and LH. In a second step, the reconstructed 236U releases are combined with 129I data from literature and oceanic and atmospheric box models are used to derive the 129I/236U and 236U/238U input functions that, for example, can be used to calculate tracer ages of Atlantic Waters in the Arctic Ocean. Our conceptual results show that the combination of 129I/236U and 236U/238U generally allows the estimation of tracer ages over the past approximately 25 yr if contributions of 236U from global fallout are considered. Finally, as a proof of concept, the new method is applied to calculate tracer ages of Arctic Ocean surface samples (collected in 2011/12) and the results are in good agreement with literature data. We conclude that the combination of 129I/236U with 236U/238U in a dual tracer approach provides a sensitive tool for the calculation of tracer ages and ventilation rates in the North Atlantic region. This article is protected by copyright. All rights reserved.

Fluxes of 238U decay series radionuclides in a dicalcium phosphate industrial plant

The production of dicalcium phosphate (DCP) is part of the phosphate industry, which has been recently included in the positive list of the NORM industries defined in the revised version of the EU-BSS (Euratom 29/96). The objective of the present work is to study specific concentrations and fluxes of (238,234)U, (230)Th, (226)Ra, (210)Pb and (210)Po at the different stages of the DCP production. Results showed highest activities of (238)U and (210)Pb were found in DCP (1500-2000 Bq kg(-1)); (230)Th and (210)Po were released together with the sludges (1600-2000 Bq kg(-1)) and (226)Ra presented particularly high activities in water (48 × 10(3) Bq m(-3)) and in the reactor scales (115 × 10(3) Bq kg(-1)). Fluxes of radionuclides showed that (238)U outflows were equally distributed between sludges (16 × 10(3) kBq h(-1)) and dicalcium phosphate (20 × 10(3) kBq h(-1)); (230)Th and (210)Po were almost entirely released in the sludges (30 × 10(3)kBq h(-1)) and the greatest (210)Pb outflow was the DCP current (25 × 10(3) kBq h(-1)). (226)Ra was mainly discharged through the water effluent (12 × 10(3) kBq h(-1)). This work highlights the importance of studying the industrial processes involving NORM, as minor changes in the production steps lead to different radionuclide distribution in the process.

Evaluation of different parameters affecting the liquid scintillation spectrometry measurement of gross alpha and beta index in water samples

Liquid scintillation spectrometry is a fast competitive technique for the simultaneous evaluation of gross alpha and beta indexes. However, the implementation of this technique should not be considered as straightforward, and the pre-concentration methods to decrease the detection limit together with quenching and alpha, and beta crossover corrections should be carefully chosen according to the needs of the laboratory. Both aspects are being approached in this work as to find an easy and robust method for alpha/beta measurement in water samples, taking into account the quenching and alpha/beta crossover interferences effects. Results showed that most of the pre-concentration methods increased the quenching in the measurement, although HNO(3) 0.05 M points to be the best solution for pre-concentration and re-dissolution of the sample as converges into low quenching and maximum recovery. Subsequently, in the measurement of water samples with different conductivities, the analysis of the raw counts to obtain gross alpha and beta indexes was carried out using different approaches to implement quenching and interference corrections. If quenching and salt content in the sample are relatively low, interference and quenching-efficiency corrections do not improve the accuracy of the results within the usual precision assumed for a result of gross alpha and beta index (25%). Special attention must be paid when corrections are applied to high quenched or saline samples and when alpha and beta activities values are different in several orders of magnitude.

Potential Releases of 129I, 236U, and Pu Isotopes from the Fukushima Dai-ichi Nuclear Power Plants to the Ocean from 2013 to 2015

After the Fukushima Dai-ichi nuclear accident, many efforts were put into the determination of the presence of 137Cs, 134Cs, 131I, and other gamma-emitting radionuclides in the ocean, but minor work was done regarding the monitoring of less volatile radionuclides, pure beta-ray emitters or simply radionuclides with very long half-lives. In this study we document the temporal evolution of 129I, 236U, and Pu isotopes (239Pu and 240Pu) in seawater sampled during four different cruises performed 2, 3, and 4 years after the accident, and we compare the results to 137Cs collected at the same stations and depths. Our results show that concentrations of 129I are systematically above the nuclear weapon test levels at stations located close to the FDNPP, with a maximum value of 790 × 107 at·kg-1, that exceeds all previously reported 129I concentrations in the Pacific Ocean. Yet, the total amount of 129I released after the accident in the time 2011-2015 was calculated from the 129I/137Cs ratio of the ongoing 137Cs releases and estimated to be about 100 g (which adds to the 1 kg released during the accident in 2011). No clear evidence of Fukushima-derived 236U and Pu isotopes has been found in this study, although further monitoring is encouraged to elucidate the origin of the highest 240Pu/239Pu atom ratio of 0.293 ± 0.028 we found close to FDNPP.

Dispersion and fate of 90Sr in the Northwestern Pacific and adjacent seas: Global fallout and the Fukushima Dai-ichi accident

The 3D compartment model POSEIDON-R was applied to the Northwestern Pacific and adjacent seas to simulate the transport and fate of (90)Sr in the period 1945-2010 and to perform a radiological assessment on the releases of (90)Sr due to the Fukushima Dai-ichi nuclear accident for the period 2011-2040. The contamination due to runoff of (90)Sr from terrestrial surfaces was taken into account using a generic predictive model. A dynamical food-chain model describes the transfer of (90)Sr to phytoplankton, zooplankton, molluscs, crustaceans, piscivorous and non-piscivorous fishes. Results of the simulations were compared with observation data on (90)Sr for the period 1955-2010 and the budget of (90)Sr activity was estimated. It was found that in the East China Sea and Yellow Sea the riverine influx was 1.5% of the ocean influx and it was important only locally. Calculated concentrations of (90)Sr in water, bottom sediment and marine organisms before and after the Fukushima Dai-ichi accident are in good agreement with available experimental measurements. The concentration of (90)Sr in seawater would return to the background levels within one year after leakages were stopped. The model predicts that the concentration of (90)Sr in fish after the Fukushima Dai-ichi accident shall return to the background concentrations only 2 years later due to the delay of the transfer throughout the food web and specific accumulation of (90)Sr. The contribution of (90)Sr to the maximal dose rate due to the FDNPP accident was three orders of magnitude less than that due to (137)Cs, and thus well below the maximum effective dose limits for the public.

Anthropogenic 236U and 129I in the Mediterranean Sea: First comprehensive distribution and constrain of their sources

The first basin-wide distribution of 236U/238U atom ratios and 129I concentrations is presented for the Mediterranean Sea. During the GEOTRACES GA04S-MedSeA expedition in 2013 seawater was collected from 10 vertical profiles covering the principal sub-basins of the Mediterranean Sea. The main objective was to understand the distributions of 236U and 129I in relation to the water masses, and to constrain their sources in this region. The 236U/238U atom ratios and the 129I concentrations ranged from (710±40)×10-12 to (2220±60)×10-12 and from (4.0±0.1)×107 to (13.8±0.3)×107at·kg-1, respectively. The results show that radionuclide-poor Atlantic Water is entering at the surface through the Strait of Gibraltar whereas comparably radionuclide-enriched Levantine Intermediate Water is sinking in the Eastern Basin and flowing westward at intermediate depths. Low radionuclide levels were found in the oldest water masses at about 1000-2000m depth in the Eastern Basin. At greater depths, waters were relatively enriched in 236U and 129I due to dense water formation occurring in both, the Eastern and Western Basins. The inventories of 236U and 129I cannot be explained only by global fallout from atmospheric nuclear bomb testings carried out in the 1950s and 1960s. We estimate that the liquid input of 236U from the nuclear reprocessing facility of Marcoule (France), via the Rhône river, was of the same order of magnitude than the contribution from global fallout, whereas liquid and gaseous releases of 129I from Marcoule were up to two orders of magnitude higher than global fallout. For both radionuclides, the contribution from the Chernobyl accident is found to be minor.