Radiological environmental monitoring of groundwater around NPP: A proposal for its assessment.

Whether a nuclear installation has radiological impact and, in that case, its extension, are the questions behind any environmental analysis of the installation along its operational life. This analysis is based on the detailed establishment of the radiological background of the area. Accordingly, the dismantling and decommissioning process (D&D) of a nuclear power plant starts with a radiological monitoring plan, which includes the radiological characterization of the area and of its surroundings. At the completion of the D&D, unrestricted use for the site will be permitted strictly in accordance with results of the radiological survey within the limits established by the local authorities. Groundwater quality is typically included in any radiological analysis since, among other reasons, a significant part of it is highly likely to end up being extracted for domestic use and hence, human consumption. While there is no regulation containing maximum activity concentration or radionuclide guidance values for water that may be destined for uses other than public consumption, if groundwater is considered a "part" of the land, dose criteria for site release can be applied. Therefore, together with the guidance levels to be established for the different radionuclides expected in the groundwater, the detection limits to be employed when performing routine radio analytical characterization procedures in the laboratory should also be provided. In this paper, we first propose a relation of the potential radionuclides to be analyzed in groundwater, together with their detection limits to be achieved when the determinations are performed in a laboratory, and subsequently, we discuss the most suitable analytical methodologies and resources that would be necessary to undertake radiological characterization plans from a practical point of view.

Uncertainty and detection limits of 241Pu determination by liquid scintillation counting (LSC).

Determination of 241Pu is an essential issue for radiation protection, as it is the precursor of some nuclides with high radiotoxicity. 241Pu is a low energy beta emitter, which makes its measurement more challenging than that of Pu alpha emitters. The most widely used method for the measurement of 241Pu is liquid scintillation counting (LSC). In this method, the assessment of Pu radiochemical yield is done by measuring the sample by alpha spectrometry before being lixiviated and measured by LSC. This double measurement affects uncertainty analysis, as well as decision threshold and detection limit, considering that both components of the total yield (radiochemical and lixiviation) should be contemplated. In this paper, and for quality assurance (QA) purposes, in-depth uncertainty and detection limit formulae for the proposed method, controlling correlations and considering all the parameters involved including chemical and lixiviation yields, have been developed. A sensitivity analysis of the uncertainty budget together with an assessment of 242Pu tracer quantity to be used, ensuring a total yield of at least 50% and a relative uncertainty of the leaching yield of at most 5%, have been carried out. In addition, an analysis of the impact of the real lixiviation yield value and its uncertainty on the results has been done. As a general conclusion, and considering the values of the parameters chosen for this work (samples of 1 g measured for 24 h by LSC), the 241Pu uncertainties range from 5% to 30% depending on the activity concentration values and the detection limits range from 14 to 30 Bq kg-1, depending on yield values. The main components of the uncertainty budget are the net 241Pu and background counts obtained in the LSC measurement for low contaminated samples while this is the case for the alpha gross count rate in LSC measurement of the alpha calibration source for highly contaminated samples. In addition, an analysis of possible interference by Pu alpha emitters in the 241Pu signal and a comparison of quench standard curves of 3H and 241Pu are also performed.

Possibilities of the use of CeBr3 scintillation detectors for the measurement of the content of radionuclides in samples for environmental monitoring.

The investigation of radioactivity in samples is an application of gamma-ray spectrometry dealing with low and very low level gamma-ray activities of different isotopes. Gamma-ray spectrometry performed in the framework of radiological environmental monitoring may be done after selective sampling processes or after a chemical purification of a sample. Both cases imply that only some specific radionuclides should contribute to the obtained spectrum. Gamma-ray spectrometry performed with medium energy resolution detectors may allow the possible distinction of their photopeaks. Therefore, a cerium bromide (CeBr3) detector can be particularly attractive for routine tasks in radiological environmental monitoring as it has a high efficiency, medium energy resolution and it can work at room temperature. This study describes the conditions under which a CeBr3 detector can serve for some routine analysis in radiological analysis of samples collected in the environment or collected by air-samplers in environmental radiological monitoring programmes.

Determining the probability of locating peaks using computerized peak-location methods in gamma-ray spectra as a function of the relative peak-area uncertainty.

The probabilities of locating peaks with a high relative peak-area uncertainty were determined empirically with nine types of peak-location software used in laboratories engaged in gamma-ray spectrometry measurements. It was found that it is not possible to locate peaks with a probability of 0.95, when they have a relative peak-area uncertainty in excess of 50%. Locating peaks at these relatively high peak-area uncertainties with a probability greater than 0.95 is only possible in the library-driven mode, where the peak positions are supposed a-priori. The deficiencies of the library-driven mode and the possibilities to improve the probabilities of locating peaks are briefly discussed.

Analysis of the use of the IAEA rapid method of 89Sr and 90Sr in milk for environmental monitoring.

Rapid methods that are used during nuclear accidents or incident situations must first be implemented and validated in radioactivity measurement laboratories, so they can be ready to provide quick answers to governments, regulatory organizations and people in such situations. As these accident situations are rare and the methods are thus not frequently used, the best way to achieve this is to use the same methods for both routine environmental monitoring and rapid or emergency situations. Before this can be done, however, an analysis of the conditions under which a rapid method could be effectively used in routine situations should be carried out. This work analyses the performance of the rapid method for the simultaneous determination of 89Sr and 90Sr in milk, published by the IAEA, and compares it with another, more conventional method used for routine environmental purposes. Through numerical calculations and considering different 89Sr and 90Sr activities, we also conducted a study to obtain the optimum values for determination parameters - such as sample mass, counting times, time lapse between measurements and background counting times - that will allow the use of the IAEA rapid method as a routine environmental one.

Validating proposed migration equation and parameters' values as a tool to reproduce and predict 137Cs vertical migration activity in Spanish soils.

This paper shows the procedure performed to validate the migration equation and the migration parameters' values presented in a previous paper (Legarda et al., 2011) regarding the migration of 137Cs in Spanish mainland soils. In this paper, this model validation has been carried out checking experimentally obtained activity concentration values against those predicted by the model. This experimental data come from the measured vertical activity profiles of 8 new sampling points which are located in northern Spain. Before testing predicted values of the model, the uncertainty of those values has been assessed with the appropriate uncertainty analysis. Once establishing the uncertainty of the model, both activity concentration values, experimental versus model predicted ones, have been compared. Model validation has been performed analyzing its accuracy, studying it as a whole and also at different depth intervals. As a result, this model has been validated as a tool to predict 137Cs behaviour in a Mediterranean environment.

Radiological characterisation and radon equilibrium factor in the outdoor air of a post-industrial urban area.

The radiological characterisation of outdoor air is always a complicated task due to the several radioactive emissions coming from the different radionuclides and also because of the very short half-lives of radionuclides in the natural radioactive series. In some places, this characterisation could result in unusual values because the natural presence of radionuclides with terrestrial origin can be modified by manmade activities. Nonetheless, this characterisation is useful not only for air quality control purposes but also because radon and its progeny in the outdoor air are the main contributors to human exposure from natural sources. In this study, we have carried out air particle sampling, followed by gamma-ray spectrometry, alpha spectrometry and beta counting determinations for this purpose. Subsequently, the outdoor air has been radiologically characterised through the obtained data and using a pre-existing analytical method to take into account the radioactive decays of short half-life radionuclides during sampling, sample preparation and measuring times. Bilbao was chosen to carry out this work. It is a medium-sized town located in northern Spain, close to the Atlantic Ocean and at sea level. This city has a recent industrial past as there were numerous steel mills and other heavy industries, including some quarries, and some open pit mines close to it, which concluded in a remediation program. So, it is a place where the air is potentially modified by manmade activities. The obtained results show that activity concentration values for long-lived radionuclides that precede radon and thoron are in the order of 10(-6) Bq m(-3) and long-lived ones after radon are around 10(-4) Bq m(-3). Thoron progeny are around 2 × 10(-2) Bq m(-3) and radon progeny are around 1.8 Bq m(-3). The mean radon equilibrium factor was 0.18. All of these values are close to the minimum UNSCEAR values, but show some variability, which highlights the importance of determining activity concentrations for each naturally occurring radionuclide and the equilibrium factor in the outdoor air.

Characteristic parameters in the measurement of (14)C of biobased diesel fuels by liquid scintillation.

The direct method based on the radiocarbon content present in modern-day materials used for the quantification of the renewable origin component in diesel has been analysed in order to establish the best sample preparation and measuring conditions that minimise the limit of detection. The scintillation cocktail and the diesel/cocktail ratio have been optimised.

Effective dose in SMAW and FCAW welding processes using rutile consumables.

The shielded metal arc welding (SMAW) and flux cored arc welding (FCAW) processes use covered electrodes and flux cored wire as consumables. Among these consumables, ones containing rutile are the most widely used, and since they have a considerable natural radioactive content, they can be considered as NORM (naturally occurring radioactive material). To calculate the effective dose on workers during their use in a conservative situation, samples of slag and aerosols and particles emitted or deposited during welding were taken and measured by gamma, alpha and beta spectrometry. An analytical method was also developed for estimating the activity concentration of radionuclides in the inhaled air. (222)Rn activity concentration was also assessed. With all these data, internal and external doses were calculated. The results show that external doses are negligible in comparison with internal ones, which do not exceed 1 mSv yr(-1), either in this conservative situation or in any other more favourable one. Radionuclides after Rn in the radioactive natural series are emitted at the same activity concentration to the atmosphere, this being around 17 times higher than that corresponding to radionuclides before Rn. Taking into account these conclusions and the analytical method developed, it can be concluded that one way to assess the activity concentration of natural radionuclides in inhaled air and hence effective doses could be the early gamma-ray spectrometry of aerosols and particles sampled during the welding process.

Effective dose in the manufacturing process of rutile covered welding electrodes.

Shielded metal arc welding using covered electrodes is the most common welding process. Sometimes the covering contains naturally occurring radioactive materials (NORMs). In Spain the most used electrodes are those covered with rutile mixed with other materials. Rutile contains some detectable natural radionuclides, so it can be considered a NORM. This paper mainly focuses on the use of MCNP (Monte Carlo N-Particle Transport Code) as a predictive tool to obtain doses in a factory which produces this type of electrode and assess the radiological impact in a specific facility after estimating the internal dose.To do this, in the facility, areas of highest radiation and positions of workers were identified, radioactive content of rutile and rutile covered electrodes was measured, and, considering a worst possible scenario, external dose at working points has been calculated using MCNP. This procedure has been validated comparing the results obtained with those from a pressurised ionisation chamber and TLD dosimeters. The internal dose has been calculated using DCAL (dose and risk calculation). The doses range between 8.8 and 394 µSv yr(-1), always lower than the effective dose limit for the public, 1 mSv yr(-1). The highest dose corresponds to the mixing area.

Map on predicted deposition of Cs-137 in Spanish soils from geostatistical analyses.

The knowledge of the distribution of (137)Cs deposition over Spanish mainland soils along with the geographical, physical and morphological terrain information enable us to know the (137)Cs background content in soil. This could be useful as a tool in a hypothetical situation of an accident involving a radioactive discharge or in soil erosion studies. A Geographic Information System (GIS) would allow the gathering of all the mentioned information. In this work, gamma measurements of (137)Cs on 34 Spanish mainland soils, rainfall data taken from 778 weather stations, soil types and geographical and physical terrain information were input into a GIS. Geostatistical techniques were applied to interpolate values of (137)Cs activity at unsampled places, obtaining prediction maps of (137)Cs deposition. Up to now, geostatistical methods have been used to model spatial continuity of data. Through semivariance and cross-covariance functions the spatial correlation of such data can be studied and described. Ordinary and simple kriging techniques were carried out to map spatial patterns of (137)Cs deposition, and ordinary and simple co-kriging were used to improve the prediction map obtained through a second related variable: namely the rainfall. To choose the best prediction map of (137)Cs deposition, the spatial dependence of the variable, the correlation coefficient and the prediction errors were evaluated using the different models previously mentioned. The best result for (137)Cs deposition map was obtained when applying the co-kriging techniques.

Uncertainties in 63Ni and 55Fe determinations using liquid scintillation counting methods.

The implementation of (63)Ni and (55)Fe determination methods in an environmental laboratory implies their validation. In this process, the uncertainties related to these methods should be analysed. In this work, the expression of the uncertainty of the results obtained using separation methods followed by liquid scintillation counting is presented. This analysis includes the consideration of uncertainties coming from the different alternatives which these methods use as well as those which are specific to the individual laboratory and the competency of its operators in applying the standard ORISE (Oak Ridge Institute for Science and Education) methods.

Inventory and vertical migration of 90Sr fallout and 137Cs/90Sr ratio in Spanish mainland soils.

In this paper the inventory of (90)Sr in 34 points distributed along the Spanish peninsular territory is presented. Obtained values range between 173 Bq/m(2) and 2047 Bq/m(2). From these data set and those (137)Cs data obtained in a previous work the (137)Cs/(90)Sr activity ratio has been established, laying this value between 0.9 and 3.6. Also the migration depth of both radionuclides has been analysed obtaining for (137)Cs an average value 57% lower than that obtained for (90)Sr. Additionally, this paper presents the results obtained in 11 sampling points in which the activity vertical profile has been measured. These profiles have been analysed to state the behaviour of strontium in soils and after, by using a convective-diffusive model, the parameters of the model which governs the vertical migration of (90)Sr in the soil, v (apparent convection velocity) and D (apparent diffusion coefficient) have been evaluated. Mean values obtained are 0.20 cm/year and 3.67 cm(2)/year, respectively.

Inventory and vertical migration of ¹³7Cs in Spanish mainland soils.

In this study the total activity of (137)Cs deposited per unit area over the Spanish peninsular territory was analysed using a 150 × 150 km(2) mesh grid, with samples taken from 29 points. The deposited activities ranged between 251 and 6074 Bq/m(2). A linear relationship was obtained between these values and the mean annual rainfall at each sampling point which allowed a map to be drawn, using GIS software, which shows the distribution of total deposited (137)Cs activity across the Spanish mainland. At twelve of these sampling points the vertical migration profile of (137)Cs was obtained. These profiles are separated into two groups with different behaviour, one of which includes clay and loam soils and the other containing sandy soils. For both groups of profiles the parameters of the convective-diffusive model, which describes the vertical migration of (137)Cs in the soil, v (apparent convection velocity) and D (apparent diffusion coefficient) were calculated.

The disequilibrium between 210Po and 210Pb in raw and drinking waters.

Many countries have to monitor and control the radioactivity in drinking waters in order to ensure compliance with the requirements of their respective regulations. Among radionuclides responsible for this radioactivity there are (210)Po and (210)Pb, which are usually not in radioactive equilibrium in waters. This paper deals with the analysis of this disequilibrium and the way that the water treatment plants affect it. To do this, (210)Po and (210)Pb activity concentrations were measured in raw and drinking water. The measurements were performed by alpha-particle spectrometry and gas flow proportional counting and the corresponding formulae for uncertainties and detection limits are presented. The values obtained show that the Po/Pb ratio is lower in surface than in ground waters. Regarding water treatment, this ratio adopts values lower in drinking water than in raw waters. In any case, for the waters analysed in this work the committed effective doses due to these radionuclides, are negligible.

Americium behaviour in plastic vessels.

The adsorption of (241)Am dissolved in water in different plastic storage vessels was determined. Three different plastics were investigated with natural and distilled waters and the retention of (241)Am by these plastics was studied. The same was done by varying vessel agitation time, vessel agitation speed, surface/volume ratio of water in the vessels and water pH. Adsorptions were measured to be between 0% and 70%. The adsorption of (241)Am is minimized with no water agitation, with PET or PVC plastics, and by water acidification.

Retention of radium from thermal waters on sand filters and adsorbents.

This study was focussed on laboratory experiences of retention of radium from one thermal water on sand filters and adsorbents, trying to find an easy method for the elimination in drinkable waters polluted with this natural radio-nuclide. A thermal water from Cantabria (Spain) was selected for this work. Retention experiences were made with columns of 35 mm of diameter containing 15 cm layers of washed river sand or 4 cm layers of zeolite A3, passing known volumes of thermal water at flows between 4 and 40 ml/min with control of the retained radium by determining the amount in the water after the treatment. The statistical analysis of data suggests that retention depends on the flow and the volume passed through the columns. As additional adsorbents were used kaolin and a clay rich in illite. Jar-test experiences were made agitating known weights of adsorbents with the selected thermal water, with addition of flocculants and determination of radium in filtrated water after the treatment. Data suggest that retention is related to the weight of adsorbent used, but important quantities of radium seem remain in solution for higher amounts of adsorbents, according to the statistical treatment of data. The elution of retained radium from columns or adsorbents, previously used in experiences, should be the aim of a future research.