I. Vallés

Removal of radionuclides in drinking water by membrane treatment using ultrafiltration, reverse osmosis and electrodialysis reversal

A pilot plant had been built to test the behaviour of ultrafiltration (UF), reverse osmosis (RO), and electrodialysis reversal (EDR) in order to improve the quality of the water supplied to Barcelona metropolitan area from the Llobregat River. This paper presents results from two studies to reduce natural radioactivity. The results from the pilot plant with four different scenarios were used to design the full-scale treatment plant built (SJD WTP). The samples taken at different steps of the treatment were analysed to determine gross alpha, gross beta and uranium activity. The results obtained revealed a significant improvement in the radiological water quality provided by both membrane techniques (RO and EDR showed removal rates higher than 60%). However, UF did not show any significant removal capacity for gross alpha, gross beta or uranium activities. RO was better at reducing the radiological parameters studied and this treatment was selected and applied at the full scale treatment plant. The RO treatment used at the SJD WTP reduced the concentration of both gross alpha and gross beta activities and also produced water of high quality with an average removal of 95% for gross alpha activity and almost 93% for gross beta activity at the treatment plant.

Natural and anthropogenic radionuclides in airborne particulate samples collected in Barcelona (Spain)

Results for naturally occurring (7)Be, (210)Pb, (40)K, (214)Bi, (214)Pb, (212)Pb, (228)Ac and (208)Tl and anthropogenic (137)Cs in airborne particulate matter in the Barcelona area during the period from January 2001 to December 2005 are presented and discussed. The (212)Pb and (208)Tl, (214)Bi and (214)Pb, (7)Be and (210)Pb radionuclide levels showed a significant correlation with each other, with correlation coefficients of 0.99, 0.78 and 0.69, respectively, suggesting similar origin/behaviour of these radionuclides in the air. Caessium-137 and Potassium-40 were transported to the air as resuspended particle from the soil. The (7)Be and (210)Pb concentrations showed similar seasonal variations, with a tendency for maximum concentrations during the summer months. An inverse relationship was observed between the (7)Be, (210)Pb, (40)K and (137)Cs concentrations and weekly rainfall, indicating washout of atmospheric aerosols carrying these radionuclides.

Natural radioactivity in drinking water in Catalonia (Spain)

A survey to study natural radioactivity in drinking water was carried out in Catalonia (northeast Spain). Approximately 800 samples of drinking water were analysed between 1986 and 1993. The samples were categorized according to origin: bottled or public supply. The samples were analysed for gross alpha, gross beta, 234U, 235U, 238U, 226Ra, 228Ra, 230Th, 232Th, 210Pb, and 210Po activity. The activity concentration for gross alpha was found to range from 0.02 to 1.75 Bq/L and for gross beta from 0.04 to 2.9 Bq/L. The gross beta activity content in the majority of the samples is due to 40K. Average concentrations of 234U, 238U, 226Ra, and 210Pb in the waters studied ranged from 10 to 100 mBq/L. Concentrations of 700 mBq/L were obtained for 234U, 960 mBq/L for226 Ra, and 1130 mBq/L for 210Pb. The highest levels of alpha radioactivity are due to the presence of granitic formations in the region. A high degree of radioactive disequilibrium was noted among members of the uranium series present in some samples of water. The 234U238U activity ratio varied between 1 and 4, and the waters with the lowest uranium activity registered the highest level of 234U238U activity ratio.

Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain).

A study is presented on the distribution of (234)U, (238)U, (235)U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261mBqL(-1). The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The (234)U/(238)U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of (234)U/(238)U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found.

Experimental analysis of the mass efficiency curve for gross alpha activity and morphological study of the residue obtained by the co-precipitation method

Gross alpha activity determination in drinking water is one of the radiological parameters that must be determined in order to decide whether further specific analyses of radionuclides in samples is required. This parameter can be determined by the co-precipitation method using a ZnS(Ag) scintillation detector or a proportional counter. The method consists of collecting all alpha emitters of interest using barium and iron as carriers as they provide more uniform and homogeneous residues than the evaporation method, especially for highly saline waters. In the course of our work, the efficiencies of the gas proportional and ZnS(Ag) detectors for alpha particle detection in water residues were studied in function of sample mass (precipitate) with residues ranging between 16.0 and 35.0mg. In addition, the structure and morphological composition of a residue collected by the co-precipitation method was studied with the aim of verifying whether the residue is a homogeneous mixture. The effect of alpha energy on the efficiency and stability of the calibration samples (mass and efficiency) was studied using (230)Th, natural uranium ((nat)U) and (241)Am radionuclides.

Activity size distributions for long-lived radon decay products in aerosols collected in Barcelona (Spain)

The activity median aerodynamic diameters (AMADs) of long-lived radon decay product ((210)Pb, (210)Po) in aerosols collected in the Barcelona area (Northeast Spain) during the period from April 2006 to February 2008 are presented. The (210)Po mean AMAD was 420 nm, while the (210)Pb mean AMAD was 500 nm. The temporal evolution of (210)Pb and (210)Po AMADs shows maxima in autumn and winter and minima in spring and summer. (210)Pb AMAD are being used to estimate the mean-residence time of atmospheric aerosols.

Validation of aerosol low-level activities by comparison with a deep underground laboratory.

The activities on air filters of the radionuclides (40)K and (137)Cs were measured in an above ground laboratory and compared with the activities measured in an underground laboratory. The average relative differences were lower than 20% for (137)Cs and (40)K. The temporal series of these radionuclides in the period 2006-2010 are also presented. These results form the baseline of these radionuclides in the studied period, and are particularly interesting because they correspond to the radioactive background in Barcelona before the Fukushima accident.

Temporal evolution of radionuclides in sludge from wastewater treatment plants

Abstract22 sludge samples were analyzed from three municipal wastewater treatment plants to assess both the occurrence and the temporal behavior of radioactivity during 8 sampling campaigns carried out over the period 2007–2009. As regards natural gamma emitters radionuclides from the natural 238U series (such as 234Th, 214Pb, 214Bi, 210Pb) and the 232Th series (such as 228Ac, 212Pb, 212Bi and 208Tl) and other natural gamma emitters such as 7Be, 210Pbu or 40K were measured. In the case of man-made radionuclides small amounts of 137Cs were found, while significant amounts of 131I were detected in some samples. Correlations were found between radionuclides with the same origin. No seasonal variation for the 238U and 232Th series was found in the studied period but 7Be and 210Pbu showed seasonal variation that was explained by the monthly rainfall. The internal and external hazard indices were calculated and the results indicate that the radiological characteristics of the sludge do not present a significant radiological risk and make them suitable for future applications.

Comparative study of calibration methods for quantification of alpha-emitting radionuclides (plutonium) by semiconductor detectors

The activity of α-emitting radionuclides is usually measured by semiconductor detectors (surface barrier or ion implanted). Overlapping and composite bands are quite common problems depending on energy differences of the radionuclides and counting source preparation. The classical approach to activity quantification is based on peak integration and, when it is used, overlapping may be overcome by a detailed study of each case, whereas composite bands can not be completely resolved. Here, spectra of the α-emitting plutonium isotopes, obtained by ion implanted semiconductor detectors, have been used to compare the classical approach with a multivariate calibration method (MVC-PLS). The study is performed at environmental activity levels (0–52 dpm). The relative errors obtained for239+240Pu activity determination, using either the classical or the MVC-PLS approach with replicates, are good enough to quantify isotopes at low level activities. The distribution of relative errors is asymmetric, with a positive component for 0–10.5 dpm subset, in the classical approach whereas it is more symmetric in the MVC-PLS method. The results show that the classical approach depends on peak overlap, whereas the MVC does not. As a whole, MVC is a more robust method than the classical approach. Composite bands were studied using the239Pu–240Pu mixture; the MVC approach did not allow individual quantification due to the lack of signal reproducibility. This instability does not affect the regular integration procedures but it is important in the deconvolution processes. The lack of reproducibility is related to the source preparation process.