Radiological characterization related to lithology and risk assessment of bottled natural mineral water

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Although natural mineral waters are exempt from monitoring for radioactive substances according to Council Directive 2013/51/EURATOM, this study focuses on the radiological characterization of natural mineral water under Spanish Royal Decree 3/2023. The water studied was taken from Catalan aquifers with different lithological characteristics (sedimentary, metamorphic, or granitic) and is sold on local markets. Moreover, radiological data on the water was correlated with its lithological origin and the health risk for different age groups was assessed. Our results showed that of the 26 natural mineral waters studied, 10 exceeded gross alpha screening value (100 mBq/L), all from granitic aquifers. Further research on natural individual radionuclides was conducted on these 10 samples. 234 U and 238 U at around 1100–1600 mBq/L. In addition, 210 Pb was found in two samples, which also presented the highest 226 Ra activity, associated with granitic bedrock and the presence of 210 Po. The annual effective dose was 179.0 and 145.9 µSv/y, exceeding 100 µSv/y mainly due to the contribution of 210 Pb > 234,238 U > 210 Po> 226 Ra, in this order. After assessing the lifetime cancer risk, these two samples were determined not to pose a health risk due to ingestion. Although no radiological monitoring is required for natural mineral water, further surveillance is recommendable. Natural mineral water bottled lithology natural radioactivity risk assessment annual effective dose Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Highlights The radiological analysis indicated that the natural mineral waters studied were generally good quality. Ten out of 26 samples exceeding the gross alpha screening value came from granitic aquifers. The highest contribution to the annual effective dose came from uranium isotopes, followed by 210 Pb. Two out of 26 samples exceeded the parametrical value for indicated dose (100 µSv/y). Introduction Access to drinking water is a human right. Water must be available, safe, and affordable for personal and domestic use (UN General Assembly, 2016 ). Generally speaking, drinking water comes from two sources: the tap and bottles. Although tap water is considered suitable for human consumption and has to meet strict quality standards, bottled water seems to be preferred by consumers worldwide, primarily for its organoleptic properties (Bouhlel, Kopke, Mina, & Smakhtin, 2023 ; Yu et al., 2020 ). Specifically, 82% of bottled waters consumed in Europe are natural mineral water (NMW) (International Atomic Energy Agency, 2023 ). Spain ranks among the top five countries in Europe for bottled water consumption (Asociación Aguas Minerales de España, 2022 ; Natural Mineral Waters Europe, 2022 ), with 21% of bottled NMW volume coming from Catalonia (north-eastern Spain). This water originates from groundwater sources and is characterized by its bacteriological health, mineral content, trace elements and other components (Manteca, 2004 ). NMW quality is assessed based on microbial, chemical, and physical parameters. Moreover, the presence of radioactive substances in NMW, generally naturally occurring radionuclides from the 238 U and 232 Th decay series transferred from bedrock, must also be considered. In Spain, Royal Decree 1798/2010 (Ministerio de la Presidencia, 2011 ) regulates the exploitation and marketing of mineral waters and bottled spring waters for human consumption. However, unlike drinking water and spring waters, NMW is exempt from assessment for radioactive substances according to Council Directive 2013/51/EURATOM. Directive 2009/54/EC (Official Journal of the European Union, 2009 ) specifies that only radio-actinological properties at the source need to be established for NMW, with no regulatory quality limit set for radioactivity. Therefore, in the absence of a regulatory framework and considering that NMW is intended for human consumption, this study assessed radioactive substances within the context of Spanish drinking water legislation, namely RD 3/2023 (Ministerio de la Presidencia, 2023 ). The legislation specifies gross alpha and gross beta screening parametrical values of 100 mBq/L and 1000 mBq/L, respectively. If these parameters are exceeded, further investigation on individual natural radionuclides ( 210 Pb, 210 Po, 224 Ra, 226 Ra, 234 U, 238 U) is necessary. The presence of radioactive substances in NMW is influenced by the geology of the water source, among other factors such as the aquifer redox conditions, weathering, seasonal precipitation variation and water residence time (Altlkulaç, Kurnaz, Turhan, & Kutucu, 2022 ; International Atomic Energy Agency, 2023 ; Tapias, Melián, Sendrós, Font, & Casas, 2022 ). Consequently, the composition of each NMW is unique depending on its source. Several studies worldwide have reported great variability in the activity of natural radionuclides in bottled water or drinking water from groundwater sources depending on aquifer conditions and lithology (Altlkulaç et al., 2022 ; Bazza, Rhiyourhi, Marhou, & Hamal, 2023 ; Borrego-Alonso, Quintana-Arnés, & Lozano, 2023 ; Chmielewska, Chalupnik, Wysocka, & Smolinski, 2020 ; Khandaker et al., 2017 ; Kinahan et al., 2020 ; Pérez-Moreno, Guerrero, Mosqueda, Gázquez, & Bolívar, 2020 ; Piñero-García, Thomas, Mantero, Forssell-Aronsson, & Isaksson, 2021 ; Slavchev et al., 2022 ; Yu et al., 2020 ). For example, water from areas dominated by granitic formations tends to exhibit higher gross alpha activity (Pérez-Moreno et al., 2020 ). In those cases, the 210 Po content in groundwater can exceed 5 mBq/L, influenced by factors like seasonal precipitation, among others, as Slavchev et al. ( 2022 ) determined in Bulgarian drinking water. Additionally, 222 Rn activity is also higher in granitic formations than in sedimentary or metamorphic rock aquifers. For example, 222 Rn activity of kBq/m 3 magnitude has been reported in Chinese and US groundwaters from granitic areas (Zhuo, Iida, & Yang, 2001 ). Although the ingestion of drinking water only contributes a small fraction of radiation to the average annual committed dose, human internal exposure must be identified and recognized. Prolonged internal exposure to natural radionuclides such as uranium, radium, lead and polonium could pose health risks. However, drinking water that results in an annual consumption of 100 µSv/y or less is not expected to give rise to detectable adverse health effects (World Health Organization, 2022 ). Therefore, annual committed dose evaluation is a useful tool for protecting consumers from radiation, identifying, and preventing water quality problems, and ensuring compliance with current legislation. Given these considerations, this study aims to contribute to a broader understanding of the radiological content in Catalan bottled mineral water. Specifically, it aims to determine gross alpha, gross beta, 222 Rn and individual natural radionuclide activity in the event that these parametrical values are exceeded, as well as the physicochemical parameters in 26 brands of bottled NMW in Catalonia (listed in the Official Journal of the European Union). Statistical analyses were conducted to explore the relationship between radiological composition and lithological origin. Finally, the annual effective dose for different age groups (infants, children, and adults) and the risk of cancer due to ingestion of NMW was evaluated. Material and methods Study area Catalonia is situated in the north-eastern Iberian Peninsula, covering an area of 32,108 km 2 with over 7.566 million inhabitants (2019). Geologically, Catalonia presents a diverse range of lithological structures. Different hydrogeological units, formed by aquifer systems, are defined within these structures, as shown in Fig. 1 . These aquifers comprise specific features in terms of hydraulics and rock composition which impart chemical components and mineralization to the groundwater. Catalonia has a great variety of aquifer types, primarily classified based on their geological unit origins. Among them, three main geological units stand out: the Pyrenean Massif, the Catalan Coastal Ranges, and the Catalan Central Basin, which are the sources of the natural mineral water bottled in Catalonia (Tapias et al., 2022 ). Table 1 presents all the natural mineral bottled water analysed in the present study, classified according to its geological unit origins. Consequently, they are grouped as granitic, metamorphic, or sedimentary rocks based on the lithology of their location. Table 1 Sample codes, aquifer type and lithology classification of natural mineral bottled water samples analysed in the present study Catalan geological units Sample code Aquifer type (Generalitat de Catalunya, 2023 ) Lithology according to (Tapias et al., 2022 ) Pyrenean Massif 1; 17 Low permeability media with local aquifers in the slates and granites of Núria-Canigó Metamorphic rocks 5; 14 -Aquifer system in the Paleozoic limestones, sandstones, and slates of Boí - La Vall Fosca -Low permeability media with local aquifers in the slates of Sort - La Seu d'Urgell 24 -Aquifers of the Devorian limestones, sandstones, and shales of Moixeró (Segre) -Low permeability environment with local aquifers in the Sort - La Seu d'Urgell slates Catalan Central Basin 15 Aquifer system in the Mesozoic limestones of the Móra depression Sedimentary rocks 16 Neogene and Quaternary detrital aquifer of Alt Camp 21 -Limestone aquifer of Tàrrega -Low permeability media with local aquifers in the limestones, marls, and sandstones of Segrià-Garrigues Catalan Coastal Ranges 2; 3; 4; 8; 10; 11; 12; 13; 19 Low permeability media with aquifers in the granites of Montseny-Guilleries Granitic rocks 6; 9; 25; 26 -Low permeability media with local aquifers in the granites of the lower Costa Brava -Neogene detrital aquifer of la Selva -Alluvial aquifer of Onyar 7 Low permeability media with local aquifers in the Paleogene marls and sandstones of Garrotxa-Pla de l'Estany Sedimentary rocks 18 Low permeability media with local aquifers in the schists, slates, and granites of Albera and Cadaqués Granitic rocks 20 Low permeability media with local aquifers in the granites and slates of La Jonquera and Roc de Frausa 22 Low permeability media with local aquifers in the schists and granites of Guilleries 23 Low permeability environment with local aquifers in the granites of the lower Costa Brava Sample collection and radiochemical methods Twenty-six samples of bottled natural mineral water (nineteen still waters and seven sparkling waters) were analysed between January 2023 and November 2023. The origin locations of the aquifers for each sample are shown in Fig. 1 . All samples were directly purchased from supermarkets and online shops during the first quarter of 2023. The sampling covered nearly all of the natural mineral water brands listed in the Official Journal of the European Union, recognized in Catalonia and updated in February 2023 (Official Journal of the European Union, 2023 ; Secretaria de Salut Pública, 2023 ). However, one mineral water brand could not be analysed because it is no longer commercially available due to source closure. Upon receipt at the laboratory, all samples were prepared and analysed. 222 Rn activity was determined first, followed by non-radioactive parameters. Electrical conductivity (EC) was measured using a Cond70 + portable conductometer (XS Instruments, Italy) and pH was assessed using a pH-meter (CRISON, Spain). The mineral composition (HCO 3 − , Ca 2+ , SiO 2 , Mg 2+ , Cl − , Na + , SO 4 − 2 ) of the water samples was obtained from the labels or determined by our team when this information was unavailable. Subsequently, the radiological parameters were analysed, including gross alpha, gross beta, 40 K, 210 Pb, 210 Po, 222 Rn, 226 Ra, 234 U and 238 U. The procedures used for their determination are outlined in Table 2 and were previously described in a research article produced by members of our laboratory (Martínez et al., 2021 ). Minimum detectable activities (MDAs), calculated according to the Curie definition, were used to estimate the method’s suitability for determining all of the radiological parameters specified in Spanish RD 3/2023 (Ministerio de la Presidencia, 2023 ). These MDAs depend on the sample volume treated, the measuring times and the chemical yields and generally ranged between 5 and 60% lower than those established in Spanish legislation. Table 2 Procedures, measurement techniques, and MDA used to perform measurements of gross alpha, gross beta, 210 Pb, 210 Po, 222 Rn, 226 Ra, 234 U and 238 U Radionuclide Sample preparation Sample volume (mL) Measurement technique Standard procedure MDA [mBq/L] Gross alpha 20 mL water, evaporation, and deposition into a planchet 20 Solid scintillation counting UNE-EN ISO 10704:2019 25 Gross beta 200 mL water, evaporation, and deposition into a planchet 200 Proportional counter UNE-EN ISO 10704:2019 40 40 K 50 mL water 50 Flame photometer (evaluated from stable potassium) Internal method 0.25 ppm 210 Pb 250 mL water, Sr resin, 4:16 mL sample/Ultima Gold™ LLT 250 Liquid scintillation counting Internal method 15 210 Po 500 mL water, iron hydroxide co-precipitation, autodeposition onto silver disc 500 Alpha spectrometry Internal method 5 222 Rn 10:10 mL water/Ultima Gold™ F 10 Liquid scintillation counting ISO 13164-4:2015 1000 226 Ra 500 mL water, barium/lead co-precipitation method 500 Solid scintillation counting Internal method 2 228 Ra 10 L water, evaporation until dry residue - Gamma spectrometry Internal method 20 234 U, 238 U 500 mL water, UTEVA, electrodeposition onto stainless steel disc 500 Alpha spectrometry ISO 13166 1 The radioanalytical procedures employed to determine gross alpha, gross beta, 210 Pb, 210 Po, 222 Rn, 226 Ra, 234 U and 238 U in water samples were externally validated through our laboratory’s participation in national and international proficiency tests at regular intervals. Results obtained, with Z-scores within the range of -1 and 1, indicated the robustness and adequacy of all methods for the intended purposes. Radiation dose assessment The total annual committed effective dose (AED) was evaluated for the samples that did not meet the parameters stipulated in Spanish legislation (gross alpha < 0.1 Bq/L, gross beta < 1 Bq/L). In those cases, AED, in µSv/y, was calculated for infants, children and adults using to the following equation: $$\:AED=\:\sum\:_{i=1}^{n}{A}_{W}\:x\:{I}_{W}\:x\:{IF}_{w}$$ 1 Where A W represents the measured activity of individual radionuclides (Bq/L) and I w is the estimated water consumption for a human over one year of age (150 L for infants, 350 L for children and 730 L for adults, respectively) (UNSCEAR, 2008). The ingestion effective dose coefficient factor (IF w ) values (Sv/Bq) used in the calculations for 210 Pb, 210 Po, 226 Ra, 234 U and 238 U were taken from the International Commission on Radiological Protection (International Comission on Radiological Protection, 1996 ). Additionally, lifetime cancer risk (LCR) was calculated using the following equation: $$\:LCR=AED\:x\:DL\:x\:RF$$ 2 Where DL represents the lifespan (79 years), and RF is the risk factor (Sv − 1 ), which is 0.05. Data handling and statistics All data were managed using Microsoft Office 365 Excel ®. Statistical analyses were conducted using Matlab 2023a (Mathworks Inc, Natick, MA, USA) and PLS Toolbox 9.3 (Eigenvector INC, Manson, WA, USA) for Matlab. Principal component analysis (PCA) was used for a multivariate analysis of the autoscaled chemical data in order to identify any relationships among the physicochemical, radiological, and lithological parameters. This technique graphically represents not the original variables, but rather new variables termed principal components (PCs), which are a linear combination of the original variables, and follow the direction of maximum variation in the data. For all quantitative assessments, concentrations below the detection limit were considered as half of the detection limit (MDA/2) for statistical analysis (U.S. EPA, 2006 ). Results and discussion Catalonia exhibits a complex hydrogeological and lithological composition, which could influence the radiological content of groundwater samples sold as bottled natural mineral water. In this section, we present the physicochemical parameters and gross alpha and gross beta activities, both used as screening parameters to assess the annual committed effective dose according to RD 3/2023 (from which NMW are exempt), determined in 26 natural mineral waters and relate them to their hydrogeological units of origin. For water samples exceeding gross alpha or gross beta, the activity of certain natural radionuclides such as 210 Pb, 210 Po, 226 Ra, 234 U and 238 U were determined to assess the potential health risk associated with ingestion of the water. Gross alpha and gross beta activity concentrations Gross alpha and gross beta activity concentrations are shown in Fig. 2A. Gross alpha activities ranged between <MDA and 2865 ± 200 mBq/L, with an average of approximately 500 mBq/L in NMW samples from granitic aquifers. 38.5% of samples (samples with codes 2, 3, 4, 8, 9, 11, 12, 13, 19 and 22) exceeded the Spanish parametrical value for gross alpha (100 mBq/L). As shown in Fig. 2B, their high alpha activity is linked to lithologic compositions mainly dominated by granitic aquifers from Girona province. It is noteworthy that some NMW samples from the same type of aquifer did not exceed the gross alpha parametrical value. Despite their granitic aquifer origin, the radiological characteristics of the samples may also be influenced by other factors, such as distance and time travelled underground before sampling, which could affect the reaction time with rocks as well as their mineral composition. Our data are consistent with previous studies in which water samples with high alpha activity concentrations originated from granitic geological areas (Martínez et al., 2021; Pérez-Moreno et al., 2020). Gross beta activity (without 40 K) ranged between <MDA and 1135 mBq/L. Only one sample (sample 13) exceeded the parametrical value. Beta emitters from the 238 U disintegration chain, which are present with high activity in this sample, are the main contributors to gross beta. NMW samples from metamorphic and sedimentary aquifers presented gross alpha and gross beta activities below their respective parametrical values. A principal component analysis was performed to summarize and elucidate the relationships between physicochemical and gross alpha and gross beta parameters in all the MNW samples tested. As shown in Fig. 3, three principal components (PCs) explained 86% of the total variance. The first PC (PC1), representing 52.48% of the total variance, is significantly correlated with dry residue, bicarbonate, chloride, sodium, potassium and conductivity (positive correlation) as well as pH (negative correlation). The second PC (PC2) accounts for 22.98% of the total variance and is significantly correlated with calcium, silica and magnesium (positive correlation) and chloride, sodium, sulphate, potassium and conductivity (negative correlation). Interestingly, the third PC (PC3) exhibits a notable correlation with gross alpha and gross beta (positive correlation). Consequently, samples positioned in the positive values of PC3 in the score plot tend to have higher values of gross alpha and gross beta. This observation is evident in Fig. 3B and 3C, where all samples exceeding the gross alpha and beta parametrical values are grouped in the positive values of PC3. Generally, samples exceeding the gross alpha and beta parametrical values tend to be characterized by high pH values and low values of all or most of the other physicochemical parameters. However, there were exceptions and not all samples with similar physicochemical composition necessarily possessed high radioactivity content. Data on 12 physicochemical parameters was collected from the commercial labels of the natural mineral water studied or identified through our own analysis. In general, the major ion composition, which determines the chemical character of each sample, varies widely in concentration among the 26 analysed NMW samples with calcium-bicarbonate and sodium-bicarbonate water types comprising the largest groups. This characteristic mineralization depends directly on the geology of the spring location and other aquifer features like residence time and depth. As an example, samples from the Montseny-Guilleries Massif, which circulated through granitic rocks, exhibited a characteristic composition, with bicarbonate as the dominant anion and a relatively low chloride content and a high silica content. On the other hand, sparkling waters associated with thermal springs (samples with codes 6, 9, 25 and 26), located predominantly in granitic rocks but also in other lithologies like volcanic or metamorphic stones, had higher mineralization, as shown in Fig. 3A (these samples are the opposite of those with high gross alpha/beta values, and therefore, as previously mentioned, they tend to have higher mineralization). Finally, a correlation matrix was performed to detect correlations between chemical components and gross alpha and beta activities. As shown in Table 3, one set of variables yielded high correlation coefficients (r > 0.75), including dry residue, conductivity, bicarbonate, chloride, sodium, and potassium, with gross alpha and gross beta presenting the highest correlation. Correlation was not determined for gross beta and potassium because, in this case, gross beta was considered without the contribution of 40 K. In the present study, natural radioactivity, expressed as the two screening parameters, did not depend primarily on the salt content of the analysed waters, indicating that NMW with high salinity are not those with higher gross alpha activity. Radionuclide release from the solid to liquid phase should be considered as a gross alpha source, including parameters like the surface roughness of the rock matrices and the irregular distribution of minerals on the surface of the rocks, among others (Bonotto, Bueno, Tessari, & Silva, 2009). Table 3 Spearman correlation matrix (significant correlations at significance level p<0.05) Gross alpha Gross beta Dry residue Bicarbonate Calcium Silica Magnesium Chloride Sodium Sulfate pH Conductivity Potassium Gross alpha 1 Gross beta 0.96 1 Dry residue -0.12 -0.16 1 Bicarbonate -0.18 -0.19 0.90 1 Calcium 0.06 0.07 0.28 0.56 1 Silica -0.12 -0.08 0.35 0.64 0.77 1 Magnesium 0.17 0.15 0.29 0.52 0.91 0.62 1 Chloride -0.04 -0.10 0.92 0.76 0.04 0.10 0.09 1 Sodium -0.17 -0.20 0.93 0.81 0.02 0.16 0.04 0.97 1 Sulfate 0.45 0.33 0.20 0.08 0.19 -0.18 0.50 0.32 0.12 1 pH 0.25 0.25 -0.74 -0.81 -0.35 -0.44 -0.33 -0.63 -0.70 0.04 1 Conductivity -0.20 -0.23 0.89 0.75 -0.07 0.09 -0.04 0.95 0.98 0.10 -0.70 1 Potassium -0.20 -0.23 0.91 0.79 -0.01 0.15 -0.01 0.96 0.99 0.08 -0.69 0.99 1 Naturally occurring radionuclides in bottled water The activity of natural radionuclides such as 234 U, 238 U, 226 Ra, 228 Ra, 210 Pb and 210 Po in NMW samples exceeding the gross alpha parametrical value (samples 2, 3, 4, 8, 9, 11, 12, 13, 19, and 22) are shown in Fig. 4 and Table 4. In general, and as can be seen in Fig. 4, considering the median values, the radionuclides 234 U and 238 U are the greatest contributors to gross alpha activity, followed by 226 Ra and 210 Po. This radionuclide contribution aligns with results obtained from the characterization of NMW samples in granitic areas from different countries such as Croatia and Sweden (Piñero-García et al., 2021). In our study, all these samples correspond to areas with predominantly granitic formations in Girona province, where rocks are known to contain high levels of 238 U disintegration chain radionuclides (Piñero-García et al., 2021). As Table 4 shows, 234 U and 238 U activities were in the range of 4.5 to 1681.2 mBq/L and 3.3 to 1433.9 mBq/L, respectively, in these NMW samples, indicating high variability despite a common origin (granitic aquifers). As stated in the literature, this great variability in activity can be attributed to the geology of the water source, among other factors such as adsorption/desorption processes in the water system, residence time, etc. (International Atomic Energy Agency, 2023). High uranium activity was determined in the samples coded 13 and 22, probably related to the enhancement of uranium leaching from host rock due to specific aquifer properties and the mineralogical composition of the granitic formations (Borrego-Alonso et al., 2023). The 234 U/ 238 U ratio ranged from 1.1 to 1.4 in these ten NMW, indicating a weak disequilibrium between the two uranium isotopes due to processes such as preferential 234 U leaching caused by alpha recoil effects, among other physicochemical processes (Dinh Chau et al., 2011). The activity of 226 Ra ranged from 1.2 to 32.1 mBq/L in granitic aquifers, which is similar to the values obtained by Pérez-Moreno et al (2020) in Spanish areas where granitic formations are predominant. In general, 226 Ra activities were below 100 mBq/L. These results are in line with the behaviour of this isotope in European water systems where low activities are associated with a relatively high uranium content (higher than 100 mBq/L) (Dinh Chau et al., 2011; Ortega, Vallés, & Serrano, 1997). This could be characteristic of young groundwaters where 238 U remains in solution while 226 Ra has not reached its secular equilibrium in the rock-water system. 228 Ra activity co-occurred in the same natural mineral waters with higher 226 Ra, although they originate from different decay chains. 228 Ra activities were below 20 mBq/L (the MDA) in samples 13 and 22. Samples with high 226 Ra activities also exhibited 210 Pb, as in the case of samples 13 and 22. This trend has been observed previously in other Catalan mineral waters from nearby areas (Ortega et al., 1997). Neither isotope is in equilibrium, likely due to 210 Pb originating from 222 Rn, which has a high diffusion rate into groundwater aquifers, or because of high 210 Pb desorption rates (Molla, Jha, Rana, & Kulkarni, 2021; Pérez-Moreno et al., 2020). In this regard, 1150.0 mBq/L of 222 Rn was determined in the sample coded 13. Low levels of 210 Po were detected in bottled water, with an average value of 6.0 ± 1.6 mBq/L. In all cases, the value was lower than the derived concentration for this isotope (100 mBq/L). As shown in Table 4, samples 13 and 22 presented the highest 210 Po activities due to their high uranium content. These results are consistent with 210 Po activity in groundwater reported in the literature (Kinahan et al., 2020; Piñero-García et al., 2021; Slavchev et al., 2022). In five samples, 210 Po/ 226 Ra exhibited a deficiency of 210 Po, probably due to its high sorption affinity with colloidal mineral particles. However, as with the case of 210 Pb/ 226 Ra, the other samples had higher related ratios, which is consistent with the arguments given above. Table 4 Activities (mBq/L) of 234,238 U, 226 Ra, 210 Po, 210 Pb, activity ratios of 234 U/ 238 U, 226 Ra/ 234 U, 210 Pb/ 226 Ra and 210 Po/ 226 Ra Sample code 234 U [mBq/L] 238 U [mBq/L] 226 Ra [mBq/L] 210 Po [mBq/L] 210 Pb [mBq/L] 234 U/ 238 U 210 Pb/ 226 Ra 210 Po/ 226 Ra 2 131.1 ± 8.0 98.7 ± 6.3 3.8 ± 0.7 1.6 ± 0.7 - 1.3 - 0.4 3 149.1 ± 8.9 141.5 ± 8.9 3.8 ± 0.9 3.5 ± 1.2 - 1.1 - 0.9 4 150.0 ± 8.9 135.8 ± 8.2 4.1 ± 1.3 3.4 ± 1.3 - 1.1 - 0.8 8 169.4 ± 9.8 130.9 ± 7.9 2.9 ± 0.7 2.2 ± 1.0 - 1.3 - 0.7 9 4.5 ± 0.9 3.3 ± 0.7 32.1 ± 2.4 1.5 ± 0.8 - 1.4 - 0.0 11 203.6 ± 11.6 151.4 ± 9.0 2.6 ± 0.6 2.8 ± 1.1 - 1.3 - 1.1 12 209.1 ± 12.5 157.1 ± 9.7 1.7 ± 0.6 1.7 ± 0.8 - 1.3 - 1.0 13 1681.2 ± 87.0 1433.9 ± 75.2 13.4 ± 1.3 20.1 ± 4.4 104.0 ± 35.0 1.2 7.8 1.5 19 389.7 ± 22.1 306.8 ± 17.8 1.2 ± 0.6 4.1 ± 1.3 - 1.3 - 3.5 22 1275.4 ± 61.1 1112.1 ± 59.4 17.1 ± 1.5 18.7 ± 3.8 90.0 ± 35.0 1.1 5.3 1.1 Estimation of annual effective dose and risk assessment We conducted a radiological health assessment in light of the results derived from the radiological characterization performed on the 26 natural mineral water samples. Gross alpha and gross beta activities were used as screening levels to check the parametric value of the indicative dose (ID), which is set at 100 µSv/y by Spanish legislation (Ministerio de la Presidencia, 2023), although NMW are exempt from these requirements. Therefore, if gross alpha and gross beta activities do not exceed 100 mBq/L and 1000 mBq/L, respectively, the ID can be considered lower than 100 µSv/y, and no further radiological study is required. This was the case of all the natural mineral waters analysed, except for samples 2, 3, 4, 8, 9, 11, 12, 13, 19 and 22, which, based on the provided information, are suitable for human consumption. On the other hand, the gross alpha screening level was exceeded in 38% of the samples. In these samples, we evaluated the annual effective dose (AED) due to the ingestion of natural radionuclides ( 210 Pb, 210 Po, 226 Ra, 234 U and 238 U) present in bottled mineral water available on the Catalan market. The samples with codes 2, 3, 4, 8, 9, 11, 12 and 19 exhibited good radiological quality, as their calculated AEDs ranged from 2.2 to 27.4 µSv/y with an average value of 13.6 µSv/y for adults, 2.5–21.3 µSv/y with an average value of 11.0 µSv/y for children and 8.5–53.9 µSv/y with an average value of 29.0 for infants. All these values are below the recommended AED (100 µSv/y), but they account for larger doses for children and infants than for adults. This is due to the fact that even though children and infants consume less water, their corresponding effective dose coefficients are higher than those for adults, resulting in a higher AED. The contribution of each natural radionuclide to the averaged AED for the previously mentioned samples was also assessed, and the results are shown in Table 5. Uranium isotopes were responsible for the highest average contribution to AED for the adult and children’s groups because they exhibit the highest activities in the analysed bottled waters. However, 210 Po is the primary contributor to the AED for the infants’ group, despite its low activity. This is related to its high effective dose coefficient due to its high radiotoxicity (University of Michigan: Environment Health and Safety, 2016). Table 5 Contribution (average values), in %, of 210 Po, 226 Ra, 234 U and 238 U to the AED AED [µSv/y] 210 Po [%] 226 Ra [%] 234 U [%] 238 U [%] Infant 29.0 35.0 7.1 27.7 30.2 Children 11.0 21.5 6.1 34.0 37.1 Adult 13.6 16.8 4.4 38.2 40.7 Among the 26 bottled natural mineral water samples analysed in the present study, two of them (samples 13 and 22) exceeded the AED (100 µSv/y) parametrical value for each specific age category, as shown in Fig. 5. Although the volume of water consumed increases from infants to adults (150 L>350 L>730 L), larger doses are associated with children and infants due to age-dependant coefficient dose factors, considering metabolism rates for different radionuclides and age groups. Adults, children and infants follow the same trend, with the AED dominated by 210 Pb and 234 U, which account for over 30% and 32% of ingestion dose, respectively, as shown in Fig. 6. Although the activities of 210 Pb are lower compared to those of uranium isotopes, the dose for lead is higher due to its higher committed effective dose per unit intake. The next most significant contributor is 238 U (25%), followed by 210 Po (11 %) and 226 Ra (2 %). The evaluation of the AED and the LCR due to the intake of natural radionuclides from samples 13 and 22 was conducted using average activity values of individual radionuclides determined in two different batches purchased six months apart. Additionally, LCR and AED parameters were estimated for adults in two scenarios. In the first scenario, the AED was assessed considering an annual water consumption per person of 730 L/year, which is the value defined in Spanish legislation (Ministerio de la Presidencia, 2023). In the second scenario, the 2022 annual consumption of MNW water per person (132 L/year) was taken to estimate the AED (Asociación Aguas Minerales de España, 2022). As Table 6 shows, AEDs from the second scenario are significantly lower than the recommended AED parametrical value set by Spanish legislation and account for 30% of the UNSCEAR estimated ingestion dose of approximately 300 µSv/y from food and drinking water (United Nations Scientific Committee on the Effects of Atomic Radiation, 2008). However, in the first scenario, AED exceeds 100 µSv/y due to the higher volume of water consumed. Unlike the other samples, samples 13 and 22 contain 210 Pb (Fig. 6). In these cases, the high dose levels received via ingestion are a consequence of the presence of lead and uranium radionuclides at high activities. The 210 Pb present in both samples is also considered a highly toxic radionuclide with a high effective dose coefficient, contributing to the increase in AED (University of Michigan: Environment Health and Safety, 2016). Finally, the LCR results obtained in both scenarios (Table 6) are lower than 10 -3 , the acceptable lifetime cancer risk (Altlkulaç et al., 2022). Table 6 Annual effective dose and life cancer risk of sample code 13 and 22, evaluated for two scenarios Scenario Sample code AED [µSv/y] LCR First (730 L/year) 13 179.0 7.1E-04 22 145.9 5.8E-04 Second (132 L/year) 13 32.4 1.3E-04 22 26.4 1.0E-04 To summarize, AED combined with LCR provides enough information to conclude that there is no radiological risk associated to the consumption of water samples 13 and 22. In this study, the health risk assessment (according to RD 3/2023 requirements) due to the ingestion of NMW was conducted in two batches of water samples to evaluate the radiological content variability due to seasonality. It is worth noting that there has been a lack of rainfall in the studied area in the past year due to climate change, which may have affected the aquifers recharge conditions, possibly leading to temporary variations in mineralization and natural radiological content in water at the source (Dinh Chau et al., 2011). Therefore, periodic radiological water surveillance assessments are recommended in order to detect the temporal variability of natural radiological content and provide the basis for possible remedial actions in terms of radiation protection and to gain a radiological perspective with regard to dose due to NMW ingestion. Conclusions This study provides detailed results on the determination of the radiological content and some of the physicochemical values of bottled natural mineral water in Catalonia. 80% of natural mineral water in Catalonia originates from granitic aquifers (Girona). The most relevant finding is that these samples were characterized by high gross alpha activity, exceeding 100 mBq/L, mainly due to the contribution of uranium radioisotopes. Occasionally, activities of more than 1000 mBq/L of 234 U and 238 U as well as 210 Pb were detected in two samples from this area. Despite the statistical analysis, no pattern could be established, and not all samples with high pH and low values of sulphate, sodium, chloride, etc. necessarily had a high radioactivity content. The total annual effective dose calculated by ingestion for adults was below the AED parametrical value stipulated in RD 3/2023 (100 µSv/y) in 92% of the natural mineral water samples analysed in this study. For the children and infant groups, although the AED was also below 100 µSv/y, it was higher than for adults. 8% of NMW samples exceeded the AED parametric value. In these situations, AED value ranged between 325–385 µSv/y for infants, 141–169 µSv/y for children and 146–179 µSv/y for adults. The main contributors to these AED values are 234,238 U> 210 Pb> 210 Po> 226 Ra. However, after combining AED with life cancer risk assessment, we concluded that there was no significant risk associated with the consumption of these two brands of natural mineral waters, although surveillance assessments in relation to radiation protection is advisable. Declarations Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have influenced the work reported in this paper. Funding This research did not receive any specific grant from funding agencies in the public, commercial, or not-for-profit sectors. Author Contribution J. M.: Conceptualization, Methodology, Formal analysis, Investigation, Writing-original draft, review & editing.A. P.: Resources, Writing – review & editing. J. R.: Formal analysis, Writing-original draft, Writing – review & editing. C. A.: Resources, Writing – review & editing, Supervision. F. B.: Resources, Writing – review & editing, Supervision. Acknowledgement The authors are grateful to the Consorci d’Aigües de Tarragona (CAT) for their invaluable collaboration.The authors would also like to thank Montserrat Novella for her assistance with sample preparation. References Altlkulaç, A., Kurnaz, A., Turhan, Ş., & Kutucu, M. (2022). Natural Radionuclides in Bottled Mineral Waters Consumed in Turkey and Their Contribution to Radiation Dose. ACS Omega , 7 (38), 34428–34435. https://doi.org/10.1021/acsomega.2c04087 Asociación Aguas Minerales de España. (2022). Memoria de actividades 2022. 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Role of lithology in the presence of natural radioactivity in drinking water samples from Tarragona province. Environmental Science and Pollution Research , 28 (29), 39333–39344. https://doi.org/10.1007/s11356-021-13470-z Ministerio de la Presidencia. (2011). Real Decreto 1798/2010, de 30 de diciembre, por el que se regula la explotación y comercialización de aguas minerales naturales y aguas de manantial envasadas para consumo humano. Retrieved from https://www.boe.es/eli/es/rd/2010/12/30/1798/con Ministerio de la Presidencia. (2023). Real Decreto 3/2023, de 10 de enero, por el que se establecen los criterios técnico-sanitarios de la calidad del agua de consumo, su control y suministro. Retrieved from https://www.boe.es/buscar/pdf/2023/BOE-A-2023-628-consolidado.pdf Molla, S., Jha, S. K., Rana, B. K., & Kulkarni, M. S. (2021). Disequilibrium of 226Ra, 210Pb, and 210Po in groundwater and soil around the Singhbhum region of Jharkhand, India. Journal of Radioanalytical and Nuclear Chemistry , 330 (3), 1243–1254. https://doi.org/10.1007/s10967-021-08055-6 Natural Mineral Waters Europe. (2022). Natural Mineral & Spring Water Statistics. Retrieved 18 December 2023, from https://naturalmineralwaterseurope.org/statistics/ Official Journal of the European Union. (2009). Directive 2009/54/EC of the European Parliament and of the Council of 18 June 2009 on the exploitation and marketing of natural mineral waters. Retrieved 13 February 2024, from https://eur-lex.europa.eu/LexUriServ/LexUriServ.do?uri=OJ:L:2009:164:0045:0058:EN:PDF Official Journal of the European Union. (2023). List of natural mineral waters recognised by Member States, United Kingdom (Northern Ireland) and EEA countries. Retrieved from https://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:52023XC0726(02) Ortega, X., Vallés, I., & Serrano, I. (1997). Natural radioactivity in drinking water in Catalonia (Spain). Environment International , 22 , 347–354. https://doi.org/10.1016/S0160-4120(96)00129-8 Pérez-Moreno, S. M., Guerrero, J. L., Mosqueda, F., Gázquez, M. J., & Bolívar, J. P. (2020). Hydrochemical behaviour of long-lived natural radionuclides in Spanish groundwaters. Catena , 191 , 1–13. https://doi.org/10.1016/j.catena.2020.104558 Piñero-García, F., Thomas, R., Mantero, J., Forssell-Aronsson, E., & Isaksson, M. (2021). Radiological impact of naturally occurring radionuclides in bottled water. Food Control , 130 , 108302. https://doi.org/10.1016/j.foodcont.2021.108302 Secretaria de Salut Pública. (2023). Aigües minerals reconegudes de Catalunya. Retrieved from https://salutweb.gencat.cat/web/.content/_ambits-actuacio/Per-perfils/Empreses-i-establiments/ambit-alimentari/llista-aigues-minerals-naturals-reconegudes-catalunya/Llista_AMN_reconegudes_Catalunya.pdf Slavchev, B., Tonev, D., Dobrev, L., Geleva, E., Veleva, B., Protohristov, H., … Dimitrova, D. (2022). Uranium and 210Po Radionuclides in Drinking Water in Southern Bulgaria and Expected Radiation Doses. Radiation Protection Dosimetry , 198 (5), 299–309. https://doi.org/10.1093/rpd/ncac039 Tapias, J. C., Melián, R., Sendrós, A., Font, X., & Casas, A. (2022). Geochemical Characterisation and Health Concerns of Mineral Bottled Waters in Catalonia (North-Eastern Spain). Water (Switzerland) , 14 (21). https://doi.org/10.3390/w14213581 U.S. EPA. (2006). Data Quality Assessment: A Reviewer’s Guide (EPA QA/G-9R). EPA/240/B-06/002 . UN General Assembly. (2016). 70/169. The human rights to safe drinking water and sanitation : resolution / adopted by the General Assembly. Retrieved 12 December 2023, from https://digitallibrary.un.org/record/821067 United Nations Scientific Committee on the Effects of Atomic Radiation. (2008). UNSCEAR 2008 Report on Sources and Effects of Ionizing Radiation . UNSCEAR 2008 report to the general assembly, with scientific annexes. UNSCEAR, vol. I . University of Michigan: Environment Health and Safety. (2016). Radionuclide toxicity classification. Retrieved 5 December 2023, from https://ehs.umich.edu/wp-content/uploads/2016/02/Table1-RadionuclideToxicityClassificaton-.pdf World Health Organization. (2022). Guidelines for drinking-water quality: fourth edition incorporating the first addendum and second addenda. Geneva. https://doi.org/10.5005/jp/books/11431_8 Yu, L., Feng, G., Liu, Q., Tang, C., Wu, B., Mao, P., & Cai, C. (2020). Assessment of natural radioactivity and consequent radiological hazard in different brands of commercialized bottled mineral water produced in China. Journal of Water and Health , 18 (4), 566–573. https://doi.org/10.2166/WH.2020.038 Zhuo, W., Iida, T., & Yang, X. (2001). Occurrence of 222Rn, 226Ra, 228Ra and U in groundwater in Fujian Province, China. Journal of Environmental Radioactivity , 53 (1), 111–120. https://doi.org/10.1016/S0265-931X(00)00108-9 Additional Declarations No competing interests reported. Cite Share Download PDF Status: Published Journal Publication published 05 Nov, 2024 Read the published version in Environmental Monitoring and Assessment → Version 1 posted Editorial decision: Revision requested 03 Sep, 2024 Reviews received at journal 20 Aug, 2024 Reviews received at journal 19 Aug, 2024 Reviewers agreed at journal 30 Jul, 2024 Reviewers agreed at journal 29 Jul, 2024 Reviewers agreed at journal 29 Jul, 2024 Reviewers agreed at journal 28 Jul, 2024 Reviewers invited by journal 27 Jul, 2024 Editor assigned by journal 18 Jul, 2024 Submission checks completed at journal 18 Jul, 2024 First submitted to journal 20 Jun, 2024 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-4610825","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":338336587,"identity":"f11cc500-db4e-410c-82f5-e8e609652e54","order_by":0,"name":"Joana Martínez","email":"","orcid":"","institution":"Departament de Química Analítica i Química Orgànica, Universitat Rovira i Virgili Unitat de Radioquímica Ambiental i Sanitaria","correspondingAuthor":false,"prefix":"","firstName":"Joana","middleName":"","lastName":"Martínez","suffix":""},{"id":338336588,"identity":"e9d9bd9d-287e-4987-9b0c-f54fd383a02c","order_by":1,"name":"Alejandra Peñalver","email":"","orcid":"","institution":"Departament de Química Analítica i Química Orgànica, Universitat Rovira i Virgili Unitat de Radioquímica Ambiental i Sanitaria","correspondingAuthor":false,"prefix":"","firstName":"Alejandra","middleName":"","lastName":"Peñalver","suffix":""},{"id":338336589,"identity":"5ffce44c-058c-48e4-9276-8856b751a928","order_by":2,"name":"Jordi Riu","email":"","orcid":"","institution":"Departament de Química Analítica i Química Orgànica, Universitat Rovira i Virgili Campus Sescelades, edifice N4","correspondingAuthor":false,"prefix":"","firstName":"Jordi","middleName":"","lastName":"Riu","suffix":""},{"id":338336590,"identity":"0628ec81-caa1-4fe0-934c-a7c76be5b1bf","order_by":3,"name":"Carme Aguilar","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA7ElEQVRIiWNgGAWjYFADZuYGBoYK0rQwArWcgXIOEKcHqIWxjQgt/O1nn274wGBnt+E4Y+PnynmH8w0OMD/8/AGPFokz6WY3ZzAkJ284zNgseXbbYcsNB9iMJfDZYsCQxnabh4E52eAwY4Nk47bDBpINPAz4tfA/Y7v9h6EepKX5Z+McsBbmH3i1SABtYWA4bAfU0ibZ2HDYgJ+Bhw2vLRI3nrHd7DE4niAJ1GLZcCzdgJ+ZzcziDB4t/P1pbDd+VFTb850/fPhmQ421ARt78+MbhKPUgCGxAc5hJqgcAuyJVDcKRsEoGAUjEQAAypZMCPxGqUIAAAAASUVORK5CYII=","orcid":"","institution":"Departament de Química Analítica i Química Orgànica, Universitat Rovira i Virgili Unitat de Radioquímica Ambiental i Sanitaria","correspondingAuthor":true,"prefix":"","firstName":"Carme","middleName":"","lastName":"Aguilar","suffix":""},{"id":338336591,"identity":"897fd8b5-5710-4495-8fe4-e325df82aa1b","order_by":4,"name":"Francesc Borrull","email":"","orcid":"","institution":"Departament de Química Analítica i Química Orgànica, Universitat Rovira i Virgili Unitat de Radioquímica Ambiental i Sanitaria","correspondingAuthor":false,"prefix":"","firstName":"Francesc","middleName":"","lastName":"Borrull","suffix":""}],"badges":[],"createdAt":"2024-06-20 09:44:16","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4610825/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4610825/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s10661-024-13353-z","type":"published","date":"2024-11-05T15:57:02+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":62659478,"identity":"49914800-e904-45d8-87e3-a6987f8da577","added_by":"auto","created_at":"2024-08-17 02:26:43","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":522090,"visible":true,"origin":"","legend":"\u003cp\u003eMap of Catalonia representing the aquifer units and locations of the origin of the samples (black dots) and the bottled mineral water samples represented by sample codes. Hydrogeological unit base map modified from (Generalitat de Catalunya, 2023)\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-4610825/v1/c05a0d1712ad95390f9d13c3.png"},{"id":62658729,"identity":"272735ab-f314-4d0c-a3a4-ae7c2b36aaef","added_by":"auto","created_at":"2024-08-17 02:18:43","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":116557,"visible":true,"origin":"","legend":"\u003cp\u003eA) Gross alpha and gross beta activity concentrations of 26 NMW samples and B) Gross alpha and gross beta related with rocks composition.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-4610825/v1/0c7bee34a0da5b1cbe72a252.png"},{"id":62658728,"identity":"2dc3f41d-8bb3-49e0-a061-94ff7f1b50db","added_by":"auto","created_at":"2024-08-17 02:18:43","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":265930,"visible":true,"origin":"","legend":"\u003cp\u003ePCA results score plot (A, B and C) and loadings (D, E and F) for the first three PCs of the PCA analysis\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-4610825/v1/a4fbe43ae1a29d0e25bd277a.png"},{"id":62659477,"identity":"13d9d452-6105-4d5d-9fa9-c74c8191ff4a","added_by":"auto","created_at":"2024-08-17 02:26:43","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":81884,"visible":true,"origin":"","legend":"\u003cp\u003eBox and whisker plot of natural radionuclide activity obtained for samples exceeding the alpha parametrical value. Lower and upper box edges correspond to the 25% and 75% percentile, respectively. The central box line is the median and the whiskers correspond to the minimum and maximum activity concentrations\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-4610825/v1/ff085f67bc4c7b3d97db0ceb.png"},{"id":62658731,"identity":"8c3565c2-6828-420d-899f-eede5e3d4016","added_by":"auto","created_at":"2024-08-17 02:18:43","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":14242,"visible":true,"origin":"","legend":"\u003cp\u003eAED, in µSv/y, due to sample 13 (a) and sample 22 (b) water consumption for infants, children and adults and individual radionuclide contribution\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-4610825/v1/e73e5c172c05f114c6f21d8a.png"},{"id":62658732,"identity":"9f53a879-5a8c-4043-9ae9-f00f06c79c03","added_by":"auto","created_at":"2024-08-17 02:18:43","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":48059,"visible":true,"origin":"","legend":"\u003cp\u003eIndividual radionuclide contribution (%) in AED due to sample 13 (a) and sample 22 (b) water consumption for adults\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-4610825/v1/30e10368d616cdffa9892e7b.png"},{"id":68749790,"identity":"42228725-e2c6-4b42-ab30-6a5b0fed81d1","added_by":"auto","created_at":"2024-11-11 16:04:52","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1830433,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4610825/v1/df37f826-1146-444e-b676-8cefd694a8ae.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Radiological characterization related to lithology and risk assessment of bottled natural mineral water","fulltext":[{"header":"Highlights","content":"\u003cul\u003e\n \u003cli\u003eThe radiological analysis indicated that the natural mineral waters studied were generally good quality.\u003c/li\u003e\n \u003cli\u003eTen out of 26 samples exceeding the gross alpha screening value came from granitic aquifers.\u003c/li\u003e\n \u003cli\u003eThe highest contribution to the annual effective dose came from uranium isotopes, followed by \u003csup\u003e210\u003c/sup\u003ePb.\u003c/li\u003e\n \u003cli\u003eTwo out of 26 samples exceeded the parametrical value for indicated dose (100 \u0026micro;Sv/y).\u003c/li\u003e\n\u003c/ul\u003e"},{"header":"Introduction","content":"\u003cp\u003eAccess to drinking water is a human right. Water must be available, safe, and affordable for personal and domestic use (UN General Assembly, \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e2016\u003c/span\u003e). Generally speaking, drinking water comes from two sources: the tap and bottles. Although tap water is considered suitable for human consumption and has to meet strict quality standards, bottled water seems to be preferred by consumers worldwide, primarily for its organoleptic properties (Bouhlel, Kopke, Mina, \u0026amp; Smakhtin, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e2023\u003c/span\u003e; Yu et al., \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Specifically, 82% of bottled waters consumed in Europe are natural mineral water (NMW) (International Atomic Energy Agency, \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). Spain ranks among the top five countries in Europe for bottled water consumption (Asociaci\u0026oacute;n Aguas Minerales de Espa\u0026ntilde;a, \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2022\u003c/span\u003e; Natural Mineral Waters Europe, \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e2022\u003c/span\u003e), with 21% of bottled NMW volume coming from Catalonia (north-eastern Spain). This water originates from groundwater sources and is characterized by its bacteriological health, mineral content, trace elements and other components (Manteca, \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e2004\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eNMW quality is assessed based on microbial, chemical, and physical parameters. Moreover, the presence of radioactive substances in NMW, generally naturally occurring radionuclides from the \u003csup\u003e238\u003c/sup\u003eU and \u003csup\u003e232\u003c/sup\u003eTh decay series transferred from bedrock, must also be considered. In Spain, Royal Decree 1798/2010 (Ministerio de la Presidencia, \u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e2011\u003c/span\u003e) regulates the exploitation and marketing of mineral waters and bottled spring waters for human consumption. However, unlike drinking water and spring waters, NMW is exempt from assessment for radioactive substances according to Council Directive 2013/51/EURATOM. Directive 2009/54/EC (Official Journal of the European Union, \u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e2009\u003c/span\u003e) specifies that only radio-actinological properties at the source need to be established for NMW, with no regulatory quality limit set for radioactivity. Therefore, in the absence of a regulatory framework and considering that NMW is intended for human consumption, this study assessed radioactive substances within the context of Spanish drinking water legislation, namely RD 3/2023 (Ministerio de la Presidencia, \u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). The legislation specifies gross alpha and gross beta screening parametrical values of 100 mBq/L and 1000 mBq/L, respectively. If these parameters are exceeded, further investigation on individual natural radionuclides (\u003csup\u003e210\u003c/sup\u003ePb, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e224\u003c/sup\u003eRa, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU, \u003csup\u003e238\u003c/sup\u003eU) is necessary.\u003c/p\u003e \u003cp\u003eThe presence of radioactive substances in NMW is influenced by the geology of the water source, among other factors such as the aquifer redox conditions, weathering, seasonal precipitation variation and water residence time (Altlkula\u0026ccedil;, Kurnaz, Turhan, \u0026amp; Kutucu, \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2022\u003c/span\u003e; International Atomic Energy Agency, \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e2023\u003c/span\u003e; Tapias, Meli\u0026aacute;n, Sendr\u0026oacute;s, Font, \u0026amp; Casas, \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). Consequently, the composition of each NMW is unique depending on its source. Several studies worldwide have reported great variability in the activity of natural radionuclides in bottled water or drinking water from groundwater sources depending on aquifer conditions and lithology (Altlkula\u0026ccedil; et al., \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2022\u003c/span\u003e; Bazza, Rhiyourhi, Marhou, \u0026amp; Hamal, \u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e2023\u003c/span\u003e; Borrego-Alonso, Quintana-Arn\u0026eacute;s, \u0026amp; Lozano, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e2023\u003c/span\u003e; Chmielewska, Chalupnik, Wysocka, \u0026amp; Smolinski, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Khandaker et al., \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e2017\u003c/span\u003e; Kinahan et al., \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; P\u0026eacute;rez-Moreno, Guerrero, Mosqueda, G\u0026aacute;zquez, \u0026amp; Bol\u0026iacute;var, \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Pi\u0026ntilde;ero-Garc\u0026iacute;a, Thomas, Mantero, Forssell-Aronsson, \u0026amp; Isaksson, \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Slavchev et al., \u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e2022\u003c/span\u003e; Yu et al., \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). For example, water from areas dominated by granitic formations tends to exhibit higher gross alpha activity (P\u0026eacute;rez-Moreno et al., \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). In those cases, the \u003csup\u003e210\u003c/sup\u003ePo content in groundwater can exceed 5 mBq/L, influenced by factors like seasonal precipitation, among others, as Slavchev et al. (\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e2022\u003c/span\u003e) determined in Bulgarian drinking water. Additionally, \u003csup\u003e222\u003c/sup\u003eRn activity is also higher in granitic formations than in sedimentary or metamorphic rock aquifers. For example, \u003csup\u003e222\u003c/sup\u003eRn activity of kBq/m\u003csup\u003e3\u003c/sup\u003e magnitude has been reported in Chinese and US groundwaters from granitic areas (Zhuo, Iida, \u0026amp; Yang, \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e2001\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eAlthough the ingestion of drinking water only contributes a small fraction of radiation to the average annual committed dose, human internal exposure must be identified and recognized. Prolonged internal exposure to natural radionuclides such as uranium, radium, lead and polonium could pose health risks. However, drinking water that results in an annual consumption of 100 \u0026micro;Sv/y or less is not expected to give rise to detectable adverse health effects (World Health Organization, \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). Therefore, annual committed dose evaluation is a useful tool for protecting consumers from radiation, identifying, and preventing water quality problems, and ensuring compliance with current legislation.\u003c/p\u003e \u003cp\u003eGiven these considerations, this study aims to contribute to a broader understanding of the radiological content in Catalan bottled mineral water. Specifically, it aims to determine gross alpha, gross beta, \u003csup\u003e222\u003c/sup\u003eRn and individual natural radionuclide activity in the event that these parametrical values are exceeded, as well as the physicochemical parameters in 26 brands of bottled NMW in Catalonia (listed in the Official Journal of the European Union). Statistical analyses were conducted to explore the relationship between radiological composition and lithological origin. Finally, the annual effective dose for different age groups (infants, children, and adults) and the risk of cancer due to ingestion of NMW was evaluated.\u003c/p\u003e"},{"header":"Material and methods","content":"\u003cp\u003eStudy area\u003c/p\u003e \u003cp\u003eCatalonia is situated in the north-eastern Iberian Peninsula, covering an area of 32,108 km\u003csup\u003e2\u003c/sup\u003e with over 7.566\u0026nbsp;million inhabitants (2019).\u003c/p\u003e \u003cp\u003eGeologically, Catalonia presents a diverse range of lithological structures. Different hydrogeological units, formed by aquifer systems, are defined within these structures, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. These aquifers comprise specific features in terms of hydraulics and rock composition which impart chemical components and mineralization to the groundwater.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eCatalonia has a great variety of aquifer types, primarily classified based on their geological unit origins. Among them, three main geological units stand out: the Pyrenean Massif, the Catalan Coastal Ranges, and the Catalan Central Basin, which are the sources of the natural mineral water bottled in Catalonia (Tapias et al., \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e presents all the natural mineral bottled water analysed in the present study, classified according to its geological unit origins. Consequently, they are grouped as granitic, metamorphic, or sedimentary rocks based on the lithology of their location.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eSample codes, aquifer type and lithology classification of natural mineral bottled water samples analysed in the present study\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"4\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCatalan geological units\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eSample code\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAquifer type (Generalitat de Catalunya, \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e2023\u003c/span\u003e)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eLithology according to (Tapias et al., \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2022\u003c/span\u003e)\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\" morerows=\"2\" rowspan=\"3\"\u003e \u003cp\u003ePyrenean Massif\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e1; 17\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLow permeability media with local aquifers in the slates and granites of N\u0026uacute;ria-Canig\u0026oacute;\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\" morerows=\"2\" rowspan=\"3\"\u003e \u003cp\u003eMetamorphic rocks\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e5; 14\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e-Aquifer system in the Paleozoic limestones, sandstones, and slates of Bo\u0026iacute; - La Vall Fosca\u003c/p\u003e \u003cp\u003e-Low permeability media with local aquifers in the slates of Sort - La Seu d'Urgell\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e24\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e-Aquifers of the Devorian limestones, sandstones, and shales of Moixer\u0026oacute; (Segre)\u003c/p\u003e \u003cp\u003e-Low permeability environment with local aquifers in the Sort - La Seu d'Urgell slates\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\" morerows=\"2\" rowspan=\"3\"\u003e \u003cp\u003eCatalan Central Basin\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAquifer system in the Mesozoic limestones of the M\u0026oacute;ra depression\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\" morerows=\"2\" rowspan=\"3\"\u003e \u003cp\u003eSedimentary rocks\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e16\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eNeogene and Quaternary detrital aquifer of Alt Camp\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e21\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e-Limestone aquifer of T\u0026agrave;rrega\u003c/p\u003e \u003cp\u003e-Low permeability media with local aquifers in the limestones, marls, and sandstones of Segri\u0026agrave;-Garrigues\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\" morerows=\"6\" rowspan=\"7\"\u003e \u003cp\u003eCatalan Coastal Ranges\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2; 3; 4; 8; 10; 11; 12; 13; 19\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLow permeability media with aquifers in the granites of Montseny-Guilleries\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eGranitic rocks\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e6; 9; 25; 26\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e-Low permeability media with local aquifers in the granites of the lower Costa Brava\u003c/p\u003e \u003cp\u003e-Neogene detrital aquifer of la Selva\u003c/p\u003e \u003cp\u003e-Alluvial aquifer of Onyar\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLow permeability media with local aquifers in the Paleogene marls and sandstones of Garrotxa-Pla de l'Estany\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eSedimentary rocks\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e18\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLow permeability media with local aquifers in the schists, slates, and granites of Albera and Cadaqu\u0026eacute;s\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\" morerows=\"3\" rowspan=\"4\"\u003e \u003cp\u003eGranitic rocks\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLow permeability media with local aquifers in the granites and slates of La Jonquera and Roc de Frausa\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e22\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLow permeability media with local aquifers in the schists and granites of Guilleries\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e23\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLow permeability environment with local aquifers in the granites of the lower Costa Brava\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eSample collection and radiochemical methods\u003c/p\u003e \u003cp\u003eTwenty-six samples of bottled natural mineral water (nineteen still waters and seven sparkling waters) were analysed between January 2023 and November 2023. The origin locations of the aquifers for each sample are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e.\u003c/p\u003e \u003cp\u003eAll samples were directly purchased from supermarkets and online shops during the first quarter of 2023. The sampling covered nearly all of the natural mineral water brands listed in the Official Journal of the European Union, recognized in Catalonia and updated in February 2023 (Official Journal of the European Union, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e2023\u003c/span\u003e; Secretaria de Salut P\u0026uacute;blica, \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). However, one mineral water brand could not be analysed because it is no longer commercially available due to source closure.\u003c/p\u003e \u003cp\u003eUpon receipt at the laboratory, all samples were prepared and analysed. \u003csup\u003e222\u003c/sup\u003eRn activity was determined first, followed by non-radioactive parameters. Electrical conductivity (EC) was measured using a Cond70\u0026thinsp;+\u0026thinsp;portable conductometer (XS Instruments, Italy) and pH was assessed using a pH-meter (CRISON, Spain). The mineral composition (HCO\u003csub\u003e3\u003c/sub\u003e\u003csup\u003e\u0026minus;\u003c/sup\u003e, Ca\u003csup\u003e2+\u003c/sup\u003e, SiO\u003csub\u003e2\u003c/sub\u003e, Mg\u003csup\u003e2+\u003c/sup\u003e, Cl\u003csup\u003e\u0026minus;\u003c/sup\u003e, Na\u003csup\u003e+\u003c/sup\u003e, SO\u003csub\u003e4\u003c/sub\u003e\u0026thinsp;\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e) of the water samples was obtained from the labels or determined by our team when this information was unavailable. Subsequently, the radiological parameters were analysed, including gross alpha, gross beta, \u003csup\u003e40\u003c/sup\u003eK, \u003csup\u003e210\u003c/sup\u003ePb, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e222\u003c/sup\u003eRn, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU. The procedures used for their determination are outlined in Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e and were previously described in a research article produced by members of our laboratory (Mart\u0026iacute;nez et al., \u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Minimum detectable activities (MDAs), calculated according to the Curie definition, were used to estimate the method\u0026rsquo;s suitability for determining all of the radiological parameters specified in Spanish RD 3/2023 (Ministerio de la Presidencia, \u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). These MDAs depend on the sample volume treated, the measuring times and the chemical yields and generally ranged between 5 and 60% lower than those established in Spanish legislation.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab2\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 2\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eProcedures, measurement techniques, and MDA used to perform measurements of gross alpha, gross beta, \u003csup\u003e210\u003c/sup\u003ePb, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e222\u003c/sup\u003eRn, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"6\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRadionuclide\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eSample preparation\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSample volume (mL)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eMeasurement technique\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003eStandard procedure\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c6\"\u003e \u003cp\u003eMDA [mBq/L]\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eGross alpha\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20 mL water, evaporation, and deposition into a planchet\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eSolid scintillation counting\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eUNE-EN ISO 10704:2019\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e25\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eGross beta\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e200 mL water, evaporation, and deposition into a planchet\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e200\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eProportional counter\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eUNE-EN ISO 10704:2019\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e40\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003csup\u003e40\u003c/sup\u003eK\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e50 mL water\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e50\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eFlame photometer (evaluated from stable potassium)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eInternal method\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e0.25 ppm\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003csup\u003e210\u003c/sup\u003ePb\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e250 mL water, Sr resin, 4:16 mL sample/Ultima Gold\u0026trade; LLT\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e250\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eLiquid scintillation counting\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eInternal method\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003csup\u003e210\u003c/sup\u003ePo\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e500 mL water, iron hydroxide co-precipitation, autodeposition onto silver disc\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e500\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eAlpha spectrometry\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eInternal method\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003csup\u003e222\u003c/sup\u003eRn\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10:10 mL water/Ultima Gold\u0026trade; F\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eLiquid scintillation counting\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eISO 13164-4:2015\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e1000\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003csup\u003e226\u003c/sup\u003eRa\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e500 mL water, barium/lead co-precipitation method\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e500\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eSolid scintillation counting\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eInternal method\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003csup\u003e228\u003c/sup\u003eRa\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10 L water, evaporation until dry residue\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e-\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eGamma spectrometry\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eInternal method\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003csup\u003e234\u003c/sup\u003eU, \u003csup\u003e238\u003c/sup\u003eU\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e500 mL water, UTEVA, electrodeposition onto stainless steel disc\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e500\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eAlpha spectrometry\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eISO 13166\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eThe radioanalytical procedures employed to determine gross alpha, gross beta, \u003csup\u003e210\u003c/sup\u003ePb, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e222\u003c/sup\u003eRn, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU in water samples were externally validated through our laboratory\u0026rsquo;s participation in national and international proficiency tests at regular intervals. Results obtained, with Z-scores within the range of -1 and 1, indicated the robustness and adequacy of all methods for the intended purposes.\u003cdiv class=\"BlockQuote\"\u003e\u003cp\u003eRadiation dose assessment\u003c/p\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003eThe total annual committed effective dose (AED) was evaluated for the samples that did not meet the parameters stipulated in Spanish legislation (gross alpha\u0026thinsp;\u0026lt;\u0026thinsp;0.1 Bq/L, gross beta\u0026thinsp;\u0026lt;\u0026thinsp;1 Bq/L). In those cases, AED, in \u0026micro;Sv/y, was calculated for infants, children and adults using to the following equation:\u003cdiv id=\"Equ1\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ1\" name=\"EquationSource\"\u003e\n$$\\:AED=\\:\\sum\\:_{i=1}^{n}{A}_{W}\\:x\\:{I}_{W}\\:x\\:{IF}_{w}$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e1\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003eWhere A\u003csub\u003eW\u003c/sub\u003e represents the measured activity of individual radionuclides (Bq/L) and I\u003csub\u003ew\u003c/sub\u003e is the estimated water consumption for a human over one year of age (150 L for infants, 350 L for children and 730 L for adults, respectively) (UNSCEAR, 2008). The ingestion effective dose coefficient factor (IF\u003csub\u003ew\u003c/sub\u003e) values (Sv/Bq) used in the calculations for \u003csup\u003e210\u003c/sup\u003ePb, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU were taken from the International Commission on Radiological Protection (International Comission on Radiological Protection, \u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e1996\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eAdditionally, lifetime cancer risk (LCR) was calculated using the following equation:\u003cdiv id=\"Equ2\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ2\" name=\"EquationSource\"\u003e\n$$\\:LCR=AED\\:x\\:DL\\:x\\:RF$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e2\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003eWhere DL represents the lifespan (79 years), and RF is the risk factor (Sv\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), which is 0.05.\u003c/p\u003e \u003cp\u003eData handling and statistics\u003c/p\u003e \u003cp\u003eAll data were managed using Microsoft Office 365 Excel \u0026reg;. Statistical analyses were conducted using Matlab 2023a (Mathworks Inc, Natick, MA, USA) and PLS Toolbox 9.3 (Eigenvector INC, Manson, WA, USA) for Matlab.\u003c/p\u003e \u003cp\u003ePrincipal component analysis (PCA) was used for a multivariate analysis of the autoscaled chemical data in order to identify any relationships among the physicochemical, radiological, and lithological parameters. This technique graphically represents not the original variables, but rather new variables termed principal components (PCs), which are a linear combination of the original variables, and follow the direction of maximum variation in the data.\u003c/p\u003e \u003cp\u003eFor all quantitative assessments, concentrations below the detection limit were considered as half of the detection limit (MDA/2) for statistical analysis (U.S. EPA, \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e2006\u003c/span\u003e).\u003c/p\u003e"},{"header":"Results and discussion","content":"\u003cp\u003eCatalonia exhibits a complex hydrogeological and lithological composition, which could influence the radiological content of groundwater samples sold as bottled natural mineral water.\u003c/p\u003e\n\u003cp\u003eIn this section, we present the physicochemical parameters and gross alpha and gross beta activities, both used as screening parameters to assess the annual committed effective dose according to RD 3/2023 (from which NMW are exempt), determined in 26 natural mineral waters and relate them to their hydrogeological units of origin. For water samples exceeding gross alpha or gross beta, the activity of certain natural radionuclides such as \u003csup\u003e210\u003c/sup\u003ePb, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU were determined to assess the potential health risk associated with ingestion of the water.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eGross alpha and gross beta activity concentrations\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eGross alpha and gross beta activity concentrations are shown in Fig. 2A. Gross alpha activities ranged between \u0026lt;MDA and 2865 \u0026plusmn; 200 mBq/L, with an average of approximately 500 mBq/L in NMW samples from granitic aquifers. 38.5% of samples (samples with codes 2, 3, 4, 8, 9, 11, 12, 13, 19 and 22) exceeded the Spanish parametrical value for gross alpha (100 mBq/L). As shown in Fig. 2B, their high alpha activity is linked to lithologic compositions mainly dominated by granitic aquifers from Girona province. It is noteworthy that some NMW samples from the same type of aquifer did not exceed the gross alpha parametrical value. Despite their granitic aquifer origin, the radiological characteristics of the samples may also be influenced by other factors, such as distance and time travelled underground before sampling, which could affect the reaction time with rocks as well as their mineral composition. Our data are consistent with previous studies in which water samples with high alpha activity concentrations originated from granitic geological areas (Mart\u0026iacute;nez et al., 2021; P\u0026eacute;rez-Moreno et al., 2020).\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eGross beta activity (without \u003csup\u003e40\u003c/sup\u003eK) ranged between \u0026lt;MDA and 1135 mBq/L. Only one sample (sample 13) exceeded the parametrical value. Beta emitters from the \u003csup\u003e238\u003c/sup\u003eU disintegration chain, which are present with high activity in this sample, are the main contributors to gross beta. NMW samples from metamorphic and sedimentary aquifers presented gross alpha and gross beta activities below their respective parametrical values.\u003c/p\u003e\n\u003cp\u003eA principal component analysis was performed to summarize and elucidate the relationships between physicochemical and gross alpha and gross beta parameters in all the MNW samples tested. As shown in Fig. 3, three principal components (PCs) explained 86% of the total variance. The first PC (PC1), representing 52.48% of the total variance, is significantly correlated with dry residue, bicarbonate, chloride, sodium, potassium and conductivity (positive correlation) as well as pH (negative correlation). The second PC (PC2) accounts for 22.98% of the total variance and is significantly correlated with calcium, silica and magnesium (positive correlation) and chloride, sodium, sulphate, potassium and conductivity (negative correlation). Interestingly, the third PC (PC3) exhibits a notable correlation with gross alpha and gross beta (positive correlation). Consequently, samples positioned in the positive values of PC3 in the score plot tend to have higher values of gross alpha and gross beta. This observation is evident in Fig. 3B and 3C, where all samples exceeding the gross alpha and beta parametrical values are grouped in the positive values of PC3. Generally, samples exceeding the gross alpha and beta parametrical values tend to be characterized by high pH values and low values of all or most of the other physicochemical parameters. However, there were exceptions and not all samples with similar physicochemical composition necessarily possessed high radioactivity content.\u003c/p\u003e\n\u003cp\u003eData on 12 physicochemical parameters was collected from the commercial labels of the natural mineral water studied or identified through our own analysis. In general, the major ion composition, which determines the chemical character of each sample, varies widely in concentration among the 26 analysed NMW samples with calcium-bicarbonate and sodium-bicarbonate water types comprising the largest groups. This characteristic mineralization depends directly on the geology of the spring location and other aquifer features like residence time and depth. As an example, samples from the Montseny-Guilleries Massif, which circulated through granitic rocks, exhibited a characteristic composition, with bicarbonate as the dominant anion and a relatively low chloride content and a high silica content. On the other hand, sparkling waters associated with thermal springs (samples with codes 6, 9, 25 and 26), located predominantly in granitic rocks but also in other lithologies like volcanic or metamorphic stones, had higher mineralization, as shown in Fig. 3A (these samples are the opposite of those with high gross alpha/beta values, and therefore, as previously mentioned, they tend to have higher mineralization).\u003c/p\u003e\n\u003cp\u003eFinally, a correlation matrix was performed to detect correlations between chemical components and gross alpha and beta activities. As shown in Table 3, one set of variables yielded high correlation coefficients (r \u0026gt; 0.75), including dry residue, conductivity, bicarbonate, chloride, sodium, and potassium, with gross alpha and gross beta presenting the highest correlation. Correlation was not determined for gross beta and potassium because, in this case, gross beta was considered without the contribution of \u003csup\u003e40\u003c/sup\u003eK. In the present study, natural radioactivity, expressed as the two screening parameters, did not depend primarily on the salt content of the analysed waters, indicating that NMW with high salinity are not those with higher gross alpha activity. Radionuclide release from the solid to liquid phase should be considered as a gross alpha source, including parameters like the surface roughness of the rock matrices and the irregular distribution of minerals on the surface of the rocks, among others (Bonotto, Bueno, Tessari, \u0026amp; Silva, 2009).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTable 3\u003c/strong\u003e Spearman correlation matrix (significant correlations at significance level p\u0026lt;0.05)\u003c/p\u003e\n\u003ctable border=\"0\" cellspacing=\"0\" cellpadding=\"0\" width=\"100%\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cem\u003e\u0026nbsp;\u003c/em\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eGross alpha\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eGross beta\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eDry residue\u0026nbsp;\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eBicarbonate\u0026nbsp;\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eCalcium\u0026nbsp;\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eSilica\u0026nbsp;\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eMagnesium\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eChloride\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eSodium\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eSulfate\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003epH\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003eConductivity\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003cem\u003ePotassium\u003c/em\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eGross alpha\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eGross beta\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.96\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eDry residue\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.12\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.16\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eBicarbonate\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.18\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.19\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.90\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eCalcium\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.06\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.07\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.28\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.56\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eSilica\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.12\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.08\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.35\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.64\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.77\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eMagnesium\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.17\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.15\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.29\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.52\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.91\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.62\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eChloride\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.04\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.10\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.92\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.76\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.04\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.10\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.09\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eSodium\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.17\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.20\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.93\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.81\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.02\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.16\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.04\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.97\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eSulfate\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.45\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.33\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.20\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.08\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.19\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.18\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.50\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.32\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.12\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003epH\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.25\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.25\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.74\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e-0.81\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.35\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.44\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.33\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.63\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.70\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.04\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003eConductivity\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.20\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.23\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.89\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.75\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.07\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.09\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.04\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.95\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.98\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.10\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.70\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003ePotassium\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.20\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.23\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.91\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.79\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.01\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.15\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.01\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"6.521739130434782%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.96\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.99\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"5.434782608695652%\" valign=\"bottom\"\u003e\n \u003cp\u003e0.08\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"4.3478260869565215%\" valign=\"bottom\"\u003e\n \u003cp\u003e-0.69\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"8.695652173913043%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e0.99\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"7.608695652173913%\" valign=\"bottom\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n\u003c/table\u003e\n\u003cp\u003eNaturally occurring radionuclides in bottled water\u0026nbsp;\u003cbr\u003eThe activity of natural radionuclides such as \u003csup\u003e234\u003c/sup\u003eU, \u003csup\u003e238\u003c/sup\u003eU, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e228\u003c/sup\u003eRa, \u003csup\u003e210\u003c/sup\u003ePb and \u003csup\u003e210\u003c/sup\u003ePo in NMW samples exceeding the gross alpha parametrical value (samples 2, 3, 4, 8, 9, 11, 12, 13, 19, and 22) are shown in Fig. 4 and Table 4. In general, and as can be seen in Fig. 4, considering the median values, the radionuclides \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU are the greatest contributors to gross alpha activity, followed by \u003csup\u003e226\u003c/sup\u003eRa and \u003csup\u003e210\u003c/sup\u003ePo. This radionuclide contribution aligns with results obtained from the characterization of NMW samples in granitic areas from different countries such as Croatia and Sweden (Pi\u0026ntilde;ero-Garc\u0026iacute;a et al., 2021). In our study, all these samples correspond to areas with predominantly granitic formations in Girona province, where rocks are known to contain high levels of \u003csup\u003e238\u003c/sup\u003eU disintegration chain radionuclides (Pi\u0026ntilde;ero-Garc\u0026iacute;a et al., 2021).\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eAs Table 4 shows, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU activities were in the range of 4.5 to 1681.2 mBq/L and 3.3 to 1433.9 mBq/L, respectively, in these NMW samples, indicating high variability despite a common origin (granitic aquifers). As stated in the literature, this great variability in activity can be attributed to the geology of the water source, among other factors such as adsorption/desorption processes in the water system, residence time, etc. (International Atomic Energy Agency, 2023). High uranium activity was determined in the samples coded 13 and 22, probably related to the enhancement of uranium leaching from host rock due to specific aquifer properties and the mineralogical composition of the granitic formations (Borrego-Alonso et al., 2023). The \u003csup\u003e234\u003c/sup\u003eU/\u003csup\u003e238\u003c/sup\u003eU ratio ranged from 1.1 to 1.4 in these ten NMW, indicating a weak disequilibrium between the two uranium isotopes due to processes such as preferential \u003csup\u003e234\u003c/sup\u003eU leaching caused by alpha recoil effects, among other physicochemical processes (Dinh Chau et al., 2011).\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe activity of \u003csup\u003e226\u003c/sup\u003eRa ranged from 1.2 to 32.1 mBq/L in granitic aquifers, which is similar to the values obtained by P\u0026eacute;rez-Moreno et al (2020) in Spanish areas where granitic formations are predominant. In general, \u003csup\u003e226\u003c/sup\u003eRa activities were below 100 mBq/L. These results are in line with the behaviour of this isotope in European water systems where low activities are associated with a relatively high uranium content (higher than 100 mBq/L) (Dinh Chau et al., 2011; Ortega, Vall\u0026eacute;s, \u0026amp; Serrano, 1997). This could be characteristic of young groundwaters where \u003csup\u003e238\u003c/sup\u003eU remains in solution while \u003csup\u003e226\u003c/sup\u003eRa has not reached its secular equilibrium in the rock-water system.\u003c/p\u003e\n\u003cp\u003e\u003csup\u003e228\u003c/sup\u003eRa activity co-occurred in the same natural mineral waters with higher \u003csup\u003e226\u003c/sup\u003eRa, although they originate from different decay chains. \u003csup\u003e228\u003c/sup\u003eRa activities were below 20 mBq/L (the MDA) in samples 13 and 22.\u003c/p\u003e\n\u003cp\u003eSamples with high \u003csup\u003e226\u003c/sup\u003eRa activities also exhibited \u003csup\u003e210\u003c/sup\u003ePb, as in the case of samples 13 and 22. This trend has been observed previously in other Catalan mineral waters from nearby areas (Ortega et al., 1997). Neither isotope is in equilibrium, likely due to \u003csup\u003e210\u003c/sup\u003ePb originating from \u003csup\u003e222\u003c/sup\u003eRn, which has a high diffusion rate into groundwater aquifers, or because of high \u003csup\u003e210\u003c/sup\u003ePb desorption rates (Molla, Jha, Rana, \u0026amp; Kulkarni, 2021; P\u0026eacute;rez-Moreno et al., 2020). In this regard, 1150.0 mBq/L of \u003csup\u003e222\u003c/sup\u003eRn was determined in the sample coded 13.\u003c/p\u003e\n\u003cp\u003eLow levels of \u003csup\u003e210\u003c/sup\u003ePo were detected in bottled water, with an average value of 6.0 \u0026plusmn; 1.6 mBq/L. In all cases, the value was lower than the derived concentration for this isotope (100 mBq/L). As shown in Table 4, samples 13 and 22 presented the highest \u003csup\u003e210\u003c/sup\u003ePo activities due to their high uranium content. These results are consistent with \u003csup\u003e210\u003c/sup\u003ePo activity in groundwater reported in the literature (Kinahan et al., 2020; Pi\u0026ntilde;ero-Garc\u0026iacute;a et al., 2021; Slavchev et al., 2022). In five samples, \u003csup\u003e210\u003c/sup\u003ePo/\u003csup\u003e226\u003c/sup\u003eRa exhibited a deficiency of \u003csup\u003e210\u003c/sup\u003ePo, probably due to its high sorption affinity with colloidal mineral particles. However, as with the case of \u003csup\u003e210\u003c/sup\u003ePb/\u003csup\u003e226\u003c/sup\u003eRa, the other samples had higher related ratios, which is consistent with the arguments given above.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTable 4\u003c/strong\u003e Activities (mBq/L) of \u003csup\u003e234,238\u003c/sup\u003eU, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e210\u003c/sup\u003ePb, activity ratios of \u003csup\u003e234\u003c/sup\u003eU/\u003csup\u003e238\u003c/sup\u003eU, \u003csup\u003e226\u003c/sup\u003eRa/\u003csup\u003e234\u003c/sup\u003eU, \u003csup\u003e210\u003c/sup\u003ePb/\u003csup\u003e226\u003c/sup\u003eRa and \u003csup\u003e210\u003c/sup\u003ePo/\u003csup\u003e226\u003c/sup\u003eRa\u003c/p\u003e\n\u003ctable border=\"0\" cellspacing=\"0\" cellpadding=\"0\" width=\"87%\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\"\u003e\n \u003cp\u003e\u003cstrong\u003eSample code\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e234\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003eU [mBq/L]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e238\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003eU [mBq/L]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e226\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003eRa [mBq/L]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e210\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003ePo [mBq/L]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e210\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003ePb \u0026nbsp;[mBq/L]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e234\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003eU/\u003csup\u003e238\u003c/sup\u003eU\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e210\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003ePb/\u003csup\u003e226\u003c/sup\u003eRa\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e210\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003ePo/\u003csup\u003e226\u003c/sup\u003eRa\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e131.1 \u0026plusmn; 8.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e98.7 \u0026plusmn; 6.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e3.8 \u0026plusmn; 0.7\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1.6 \u0026plusmn; 0.7\u0026nbsp;\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e0.4\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e3\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e149.1 \u0026plusmn; 8.9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e141.5 \u0026plusmn; 8.9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\" valign=\"bottom\"\u003e\n \u003cp\u003e3.8 \u0026plusmn; 0.9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e3.5 \u0026plusmn; 1.2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e0.9\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e4\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e150.0 \u0026plusmn; 8.9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e135.8 \u0026plusmn; 8.2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e4.1 \u0026plusmn; 1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e3.4 \u0026plusmn; 1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e0.8\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e8\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e169.4 \u0026plusmn; 9.8\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e\u0026nbsp;130.9 \u0026plusmn; 7.9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e2.9 \u0026plusmn; 0.7\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e2.2 \u0026plusmn; 1.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e0.7\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e9\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e4.5 \u0026plusmn; 0.9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e3.3 \u0026plusmn; 0.7\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e32.1 \u0026plusmn; 2.4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1.5 \u0026plusmn; 0.8\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e0.0\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e11\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e203.6 \u0026plusmn; 11.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e151.4 \u0026plusmn; 9.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e2.6 \u0026plusmn; 0.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e2.8 \u0026plusmn; 1.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e1.1\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e12\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e209.1 \u0026plusmn; 12.5\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e157.1 \u0026plusmn; 9.7\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1.7 \u0026plusmn; 0.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1.7 \u0026plusmn; 0.8\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e1.0\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e13\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1681.2 \u0026plusmn; 87.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1433.9 \u0026plusmn; 75.2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e13.4 \u0026plusmn; 1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e20.1 \u0026plusmn; 4.4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e104.0 \u0026plusmn; 35.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e7.8\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e1.5\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e19\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e389.7 \u0026plusmn; 22.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e306.8 \u0026plusmn; 17.8\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1.2 \u0026plusmn; 0.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e4.1 \u0026plusmn; 1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e3.5\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.602150537634408%\" valign=\"bottom\"\u003e\n \u003cp\u003e\u003cstrong\u003e22\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1275.4 \u0026plusmn; 61.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e1112.1 \u0026plusmn; 59.4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e17.1 \u0026plusmn; 1.5\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e18.7 \u0026plusmn; 3.8\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"9.67741935483871%\"\u003e\n \u003cp\u003e90.0 \u0026plusmn; 35.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"12.903225806451612%\"\u003e\n \u003cp\u003e1.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e5.3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.053763440860216%\"\u003e\n \u003cp\u003e1.1\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n\u003c/table\u003e\n\u003cp\u003eEstimation of annual effective dose and risk assessment\u003c/p\u003e\n\u003cp\u003eWe conducted a radiological health assessment in light of the results derived from the radiological characterization performed on the 26 natural mineral water samples.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eGross alpha and gross beta activities were used as screening levels to check the parametric value of the indicative dose (ID), which is set at 100 \u0026micro;Sv/y by Spanish legislation\u0026nbsp;(Ministerio de la Presidencia, 2023), although NMW are exempt from these requirements. Therefore, if gross alpha and gross beta activities do not exceed 100 mBq/L and 1000 mBq/L, respectively, the ID can be considered lower than 100 \u0026micro;Sv/y, and no further radiological study is required. This was the case of all the natural mineral waters analysed, except for samples 2, 3, 4, 8, 9, 11, 12, 13, 19 and 22, which, based on the provided information, are suitable for human consumption.\u003c/p\u003e\n\u003cp\u003eOn the other hand, the gross alpha screening level was exceeded in 38% of the samples. In these samples, we evaluated the annual effective dose (AED) due to the ingestion of natural radionuclides (\u003csup\u003e210\u003c/sup\u003ePb, \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU) present in bottled mineral water available on the Catalan market. The samples with codes 2, 3, 4, 8, 9, 11, 12 and 19 exhibited good radiological quality, as their calculated AEDs ranged from 2.2 to 27.4 \u0026micro;Sv/y with an average value of 13.6 \u0026micro;Sv/y for adults, 2.5\u0026ndash;21.3 \u0026micro;Sv/y with an average value of 11.0 \u0026micro;Sv/y for children and 8.5\u0026ndash;53.9 \u0026micro;Sv/y with an average value of 29.0 for infants. All these values are below the recommended AED (100 \u0026micro;Sv/y), but they account for larger doses for children and infants than for adults. This is due to the fact that even though children and infants consume less water, their corresponding effective dose coefficients are higher than those for adults, resulting in a higher AED. The contribution of each natural radionuclide to the averaged AED for the previously mentioned samples was also assessed, and the results are shown in Table 5. Uranium isotopes were responsible for the highest average contribution to AED for the adult and children\u0026rsquo;s groups because they exhibit the highest activities in the analysed bottled waters. However, \u003csup\u003e210\u003c/sup\u003ePo is the primary contributor to the AED for the infants\u0026rsquo; group, despite its low activity. This is related to its high effective dose coefficient due to its high radiotoxicity\u0026nbsp;(University of Michigan: Environment Health and Safety, 2016).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTable 5\u003c/strong\u003e Contribution (average values), in %, of \u003csup\u003e210\u003c/sup\u003ePo, \u003csup\u003e226\u003c/sup\u003eRa, \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU to the AED\u003c/p\u003e\n\u003cdiv align=\"\"\u003e\n \u003ctable border=\"0\" cellspacing=\"0\" cellpadding=\"0\" width=\"488\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u0026nbsp;\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.637860082304528%\"\u003e\n \u003cp\u003e\u003cstrong\u003eAED [\u0026micro;Sv/y]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e210\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003ePo [%]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e226\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003eRa [%]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e234\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003eU [%]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u003csup\u003e238\u003c/sup\u003e\u003c/strong\u003e\u003cstrong\u003eU [%]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u003cstrong\u003eInfant\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.637860082304528%\"\u003e\n \u003cp\u003e29.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e35.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e7.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e27.7\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e30.2\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u003cstrong\u003eChildren\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.637860082304528%\"\u003e\n \u003cp\u003e11.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e21.5\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e6.1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e34.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e37.1\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e\u003cstrong\u003eAdult\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.637860082304528%\"\u003e\n \u003cp\u003e13.6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e16.8\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e4.4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e38.2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.872427983539094%\"\u003e\n \u003cp\u003e40.7\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n \u003c/table\u003e\n\u003c/div\u003e\n\u003cp\u003e\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eAmong the 26 bottled natural mineral water samples analysed in the present study, two of them (samples 13 and 22) exceeded the AED (100 \u0026micro;Sv/y) parametrical value for each specific age category, as shown in Fig. 5. Although the volume of water consumed increases from infants to adults (150 L\u0026gt;350 L\u0026gt;730 L), larger doses are associated with children and infants due to age-dependant coefficient dose factors, considering metabolism rates for different radionuclides and age groups. Adults, children and infants follow the same trend, with the AED dominated by \u003csup\u003e210\u003c/sup\u003ePb and \u003csup\u003e234\u003c/sup\u003eU, which account for over 30% and 32% of ingestion dose, respectively, as shown in Fig. 6. Although the activities of \u003csup\u003e210\u003c/sup\u003ePb are lower compared to those of uranium isotopes, the dose for lead is higher due to its higher committed effective dose per unit intake. The next most significant contributor is \u003csup\u003e238\u003c/sup\u003eU (25%), followed by \u003csup\u003e210\u003c/sup\u003ePo (11 %) and \u003csup\u003e226\u003c/sup\u003eRa (2 %).\u003c/p\u003e\n\u003cp\u003eThe evaluation of the AED and the LCR due to the intake of natural radionuclides from samples 13 and 22 was conducted using average activity values of individual radionuclides determined in two different batches purchased six months apart. Additionally, LCR and AED parameters were estimated for adults in two scenarios. In the first scenario, the AED was assessed considering an annual water consumption per person of 730 L/year, which is the value defined in Spanish legislation (Ministerio de la Presidencia, 2023). In the second scenario, the 2022 annual consumption of MNW water per person (132 L/year) was taken to estimate the AED (Asociaci\u0026oacute;n Aguas Minerales de Espa\u0026ntilde;a, 2022). As Table 6 shows, AEDs from the second scenario are significantly lower than the recommended AED parametrical value set by Spanish legislation and account for 30% of the UNSCEAR estimated ingestion dose of approximately 300 \u0026micro;Sv/y from food and drinking water (United Nations Scientific Committee on the Effects of Atomic Radiation, 2008). However, in the first scenario, AED exceeds 100 \u0026micro;Sv/y due to the higher volume of water consumed. Unlike the other samples, samples 13 and 22 contain \u003csup\u003e210\u003c/sup\u003ePb (Fig. 6). In these cases, the high dose levels received via ingestion are a consequence of the presence of lead and uranium radionuclides at high activities. The \u003csup\u003e210\u003c/sup\u003ePb present in both samples is also considered a highly toxic radionuclide with a high effective dose coefficient, contributing to the increase in AED\u0026nbsp;(University of Michigan: Environment Health and Safety, 2016). Finally, the LCR results obtained in both scenarios (Table 6) are lower than 10\u003csup\u003e-3\u003c/sup\u003e, the acceptable lifetime cancer risk (Altlkula\u0026ccedil; et al., 2022).\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTable 6\u003c/strong\u003e Annual effective dose and life cancer risk of sample code 13 and 22, evaluated for two scenarios\u003c/p\u003e\n\u003cdiv align=\"\"\u003e\n \u003ctable border=\"0\" cellspacing=\"0\" cellpadding=\"0\" width=\"65%\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd width=\"39.795918367346935%\"\u003e\n \u003cp\u003e\u003cstrong\u003eScenario\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"26.53061224489796%\"\u003e\n \u003cp\u003e\u003cstrong\u003eSample code\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.306122448979592%\"\u003e\n \u003cp\u003e\u003cstrong\u003eAED [\u0026micro;Sv/y]\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"18.367346938775512%\"\u003e\n \u003cp\u003e\u003cstrong\u003eLCR\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"39.795918367346935%\" rowspan=\"2\"\u003e\n \u003cp\u003e\u003cstrong\u003eFirst (730 L/year)\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"26.53061224489796%\"\u003e\n \u003cp\u003e\u003cstrong\u003e13\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.306122448979592%\"\u003e\n \u003cp\u003e179.0\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"18.367346938775512%\"\u003e\n \u003cp\u003e7.1E-04\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"44.067796610169495%\"\u003e\n \u003cp\u003e\u003cstrong\u003e22\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"25.423728813559322%\"\u003e\n \u003cp\u003e145.9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"30.508474576271187%\"\u003e\n \u003cp\u003e5.8E-04\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"39.795918367346935%\" rowspan=\"2\"\u003e\n \u003cp\u003e\u003cstrong\u003eSecond (132 L/year)\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"26.53061224489796%\"\u003e\n \u003cp\u003e\u003cstrong\u003e13\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"15.306122448979592%\"\u003e\n \u003cp\u003e32.4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"18.367346938775512%\"\u003e\n \u003cp\u003e1.3E-04\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"44.067796610169495%\"\u003e\n \u003cp\u003e\u003cstrong\u003e22\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"25.423728813559322%\"\u003e\n \u003cp\u003e26.4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"30.508474576271187%\"\u003e\n \u003cp\u003e1.0E-04\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n \u003c/table\u003e\n\u003c/div\u003e\n\u003cp\u003eTo summarize, AED combined with LCR provides enough information to conclude that there is no radiological risk associated to the consumption of water samples 13 and 22. In this study, the health risk assessment (according to RD 3/2023 requirements) due to the ingestion of NMW was conducted in two batches of water samples to evaluate the radiological content variability due to seasonality. It is worth noting that there has been a lack of rainfall in the studied area in the past year due to climate change, which may have affected the aquifers recharge conditions, possibly leading to temporary variations in mineralization and natural radiological content in water at the source (Dinh Chau et al., 2011). Therefore, periodic radiological water surveillance assessments are recommended in order to detect the temporal variability of natural radiological content and provide the basis for possible remedial actions in terms of radiation protection and to gain a radiological perspective with regard to dose due to NMW ingestion.\u0026nbsp;\u003c/p\u003e"},{"header":"Conclusions","content":"\u003cp\u003eThis study provides detailed results on the determination of the radiological content and some of the physicochemical values of bottled natural mineral water in Catalonia. 80% of natural mineral water in Catalonia originates from granitic aquifers (Girona). The most relevant finding is that these samples were characterized by high gross alpha activity, exceeding 100 mBq/L, mainly due to the contribution of uranium radioisotopes. Occasionally, activities of more than 1000 mBq/L of \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU as well as \u003csup\u003e210\u003c/sup\u003ePb were detected in two samples from this area. Despite the statistical analysis, no pattern could be established, and not all samples with high pH and low values of sulphate, sodium, chloride, etc. necessarily had a high radioactivity content.\u003c/p\u003e \u003cp\u003eThe total annual effective dose calculated by ingestion for adults was below the AED parametrical value stipulated in RD 3/2023 (100 \u0026micro;Sv/y) in 92% of the natural mineral water samples analysed in this study. For the children and infant groups, although the AED was also below 100 \u0026micro;Sv/y, it was higher than for adults. 8% of NMW samples exceeded the AED parametric value. In these situations, AED value ranged between 325\u0026ndash;385 \u0026micro;Sv/y for infants, 141\u0026ndash;169 \u0026micro;Sv/y for children and 146\u0026ndash;179 \u0026micro;Sv/y for adults. The main contributors to these AED values are \u003csup\u003e234,238\u003c/sup\u003eU\u0026gt;\u003csup\u003e210\u003c/sup\u003ePb\u0026gt;\u003csup\u003e210\u003c/sup\u003ePo\u0026gt;\u003csup\u003e226\u003c/sup\u003eRa. However, after combining AED with life cancer risk assessment, we concluded that there was no significant risk associated with the consumption of these two brands of natural mineral waters, although surveillance assessments in relation to radiation protection is advisable.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e \u003ch2\u003eDeclaration of competing interest\u003c/h2\u003e \u003cp\u003eThe authors declare that they have no known competing financial interests or personal relationships that could have influenced the work reported in this paper.\u003c/p\u003e \u003c/p\u003e\u003ch2\u003eFunding\u003c/h2\u003e \u003cp\u003eThis research did not receive any specific grant from funding agencies in the public, commercial, or not-for-profit sectors.\u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eJ. M.: Conceptualization, Methodology, Formal analysis, Investigation, Writing-original draft, review \u0026amp; editing.A. P.: Resources, Writing \u0026ndash; review \u0026amp; editing. J. R.: Formal analysis, Writing-original draft, Writing \u0026ndash; review \u0026amp; editing. C. A.: Resources, Writing \u0026ndash; review \u0026amp; editing, Supervision. F. B.: Resources, Writing \u0026ndash; review \u0026amp; editing, Supervision.\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eThe authors are grateful to the Consorci d\u0026rsquo;Aig\u0026uuml;es de Tarragona (CAT) for their invaluable collaboration.The authors would also like to thank Montserrat Novella for her assistance with sample preparation.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n \u003cli\u003eAltlkula\u0026ccedil;, A., Kurnaz, A., Turhan, Ş., \u0026amp; Kutucu, M. (2022). 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Occurrence of 222Rn, 226Ra, 228Ra and U in groundwater in Fujian Province, China. \u003cem\u003eJournal of Environmental Radioactivity\u003c/em\u003e, \u003cem\u003e53\u003c/em\u003e(1), 111\u0026ndash;120. https://doi.org/10.1016/S0265-931X(00)00108-9\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"environmental-monitoring-and-assessment","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"emas","sideBox":"Learn more about [Environmental Monitoring and Assessment](http://link.springer.com/journal/10661)","snPcode":"10661","submissionUrl":"https://submission.nature.com/new-submission/10661/3","title":"Environmental Monitoring and Assessment","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Natural mineral water, bottled, lithology, natural radioactivity, risk assessment, annual effective dose","lastPublishedDoi":"10.21203/rs.3.rs-4610825/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4610825/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe enhancement of natural radioactivity in groundwater, specifically in natural mineral water, is related to the lithological formations through which water bodies or courses pass. Although natural mineral waters are exempt from monitoring for radioactive substances according to Council Directive 2013/51/EURATOM, this study focuses on the radiological characterization of natural mineral water under Spanish Royal Decree 3/2023. The water studied was taken from Catalan aquifers with different lithological characteristics (sedimentary, metamorphic, or granitic) and is sold on local markets. Moreover, radiological data on the water was correlated with its lithological origin and the health risk for different age groups was assessed. Our results showed that of the 26 natural mineral waters studied, 10 exceeded gross alpha screening value (100 mBq/L), all from granitic aquifers. Further research on natural individual radionuclides was conducted on these 10 samples. \u003csup\u003e234\u003c/sup\u003eU and \u003csup\u003e238\u003c/sup\u003eU at around 1100–1600 mBq/L. In addition, \u003csup\u003e210\u003c/sup\u003ePb was found in two samples, which also presented the highest \u003csup\u003e226\u003c/sup\u003eRa activity, associated with granitic bedrock and the presence of \u003csup\u003e210\u003c/sup\u003ePo. The annual effective dose was 179.0 and 145.9 µSv/y, exceeding 100 µSv/y mainly due to the contribution of \u003csup\u003e210\u003c/sup\u003ePb \u0026gt;\u003csup\u003e234,238\u003c/sup\u003eU \u0026gt;\u003csup\u003e210\u003c/sup\u003ePo\u0026gt;\u003csup\u003e226\u003c/sup\u003eRa, in this order. After assessing the lifetime cancer risk, these two samples were determined not to pose a health risk due to ingestion. Although no radiological monitoring is required for natural mineral water, further surveillance is recommendable.\u003c/p\u003e","manuscriptTitle":"Radiological characterization related to lithology and risk assessment of bottled natural mineral water","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-08-17 02:18:38","doi":"10.21203/rs.3.rs-4610825/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2024-09-03T17:05:59+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-08-20T16:15:24+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-08-20T01:06:01+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"147146254390273766600492107199997990042","date":"2024-07-30T10:26:38+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"60009275742549370916388535746466930664","date":"2024-07-30T01:40:29+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"189584813580859507132687131605868814907","date":"2024-07-29T08:05:49+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"148078015989792612432612019751378496674","date":"2024-07-28T08:06:27+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2024-07-27T19:04:20+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-07-18T20:19:40+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2024-07-18T20:19:15+00:00","index":"","fulltext":""},{"type":"submitted","content":"Environmental Monitoring and Assessment","date":"2024-06-20T09:42:33+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"environmental-monitoring-and-assessment","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"emas","sideBox":"Learn more about [Environmental Monitoring and Assessment](http://link.springer.com/journal/10661)","snPcode":"10661","submissionUrl":"https://submission.nature.com/new-submission/10661/3","title":"Environmental Monitoring and Assessment","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"66505298-0d55-4a12-bd3f-b3b16cf67058","owner":[],"postedDate":"August 17th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2024-11-11T15:59:01+00:00","versionOfRecord":{"articleIdentity":"rs-4610825","link":"https://doi.org/10.1007/s10661-024-13353-z","journal":{"identity":"environmental-monitoring-and-assessment","isVorOnly":false,"title":"Environmental Monitoring and Assessment"},"publishedOn":"2024-11-05 15:57:02","publishedOnDateReadable":"November 5th, 2024"},"versionCreatedAt":"2024-08-17 02:18:38","video":"","vorDoi":"10.1007/s10661-024-13353-z","vorDoiUrl":"https://doi.org/10.1007/s10661-024-13353-z","workflowStages":[]},"version":"v1","identity":"rs-4610825","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4610825","identity":"rs-4610825","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}