The Physico-Chemical and Radionuclide Characterisation of Soil near a Future Radioactive Waste Management Centre
by
, , , , , ,
Tomislav Bituh
1
,
Branko Petrinec
1,2,*,
Martina Novosel
3,
Dinko Babić
1,
Davor Rašeta
4,
Iva Hrelja
3,
Marija Galić
3,
Aleksandra Perčin
3,
Ivan Širić
3,
Ivica Kisić
3,
Andrea Rapić
4 and
Željka Zgorelec
3
1
Division of Radiation Protection, Institute for Medical Research and Occupational Health, Ksaverska Cesta 2, HR-10000 Zagreb, Croatia
2
Faculty of Dental Medicine and Health, Josip Juraj Strossmayer University of Osijek, Crkvena 21, HR-31000 Osijek, Croatia
3
Faculty of Agriculture, University of Zagreb, Svetošimunska 25, HR-10000 Zagreb, Croatia
4
Fund for Financing the Decommissioning of the Krško Nuclear Power Plant, The Disposal of Krško NPP Radioactive Waste and Spent Nuclear Fuel, Ulica Vjekoslava Heinzela 70A, HR-10000 Zagreb, Croatia
*
Author to whom correspondence should be addressed.
Environments 2025, 12(4), 121; https://doi.org/10.3390/environments12040121
Submission received: 6 March 2025
/
Revised: 31 March 2025
/
Accepted: 11 April 2025
/
Published: 15 April 2025
Abstract
:A future radioactive waste management centre is under development in central Croatia. One of the activities in the centre’s development was to monitor environmental radioactivity before the disposal of radioactive materials. Part of the monitoring programme focused on soil characterisation in the municipality (total area 1308 km2) surrounding the centre, where about 40% of the soil is today used in organic farming. The study included a physico-chemical and radionuclide characterisation of the soil as well as ambient dose rate measurements. The aim of this study was to investigate how the physical and chemical composition of soil affects the concentration of radionuclides 238U, 40K, and 137Cs in soil, based on the measured radionuclide concentrations and values of selected soil parameters. Additionally, the ambient equivalent dose rate H*(10)/t was measured and the annual effective dose was calculated for the average person living in the area of interest. The observed ranges of radionuclide concentrations in the soil samples were: 9–72 Bq/kg for 238U, 65–823 Bq/kg for 40K, and 4–80 Bq/kg for 137Cs. Ambient dose equivalent rate measurements were in the range of 52–130 nSv/h. The highest measured values were in correlation with higher 238U activity concentrations in these parts of the investigated area. The results of this study showed that 238U had a significant correlation with pH; plant available P; sand, silt, and clay content; hydrolytic acidity; CaCO3; total carbon, organic matter, and total inorganic and organic carbon; and concentrations of Al, Si, Fe, Ca, Ti, K, Rb, Zr, Nb, Y, Sr, Th, and W. 40K showed a significant correlation with pH, sand content, hydrolytic acidity, total hydrogen, total nitrogen, CaCO3, total carbon, total inorganic carbon, and concentrations of Al, Si, Fe, Ca, Ti, Rb, Zr, Nb, P, Y, Zn, and Th. 137Cs showed a significant correlation with silt content, total nitrogen, and Si concentration.
1. Introduction
Radioactive waste management is a critical component of nuclear energy and medicine. Proper management methods are necessary to ensure that environmental and human health risks are minimised. Radioactive waste management sites are carefully selected based on geological and ecological assessments to prevent the contamination of natural resources [1]. A future radioactive waste management site, amongst other assessments, must be evaluated thoroughly through radionuclide analyses of the surrounding soil to determine its suitability [2,3]. Measurements discussed in this study are a first step in planning and designing long-term storage of radioactive waste.
Radionuclides can be found in all environmental media. They are found in air, water and soil, but also in living organisms, including humans, while the highest concentrations are found in rocks, Earth’s interior, and soil [4]. In addition to naturally occurring radionuclides, with the development of technology and industry, radionuclides originating from human activity have also appeared in nature. Their biggest problem related to radionuclides is their long residence time in the environment. As radionuclides decay, new radionuclides can be produced, and at the end of each decay sequence, there is an isotope with a stable atomic nucleus [5]. In terms of origin, a distinction is made between natural and anthropogenic radionuclides. In this work, the concentrations of 238U and 40K (primordial and naturally occurring) as well as of anthropogenic 137Cs were determined.
All uranium isotopes are unstable and radioactive, emitting alpha radiation. 238U is the most abundant (99.3%) and has an extremely long half-life of 4.5 billion years. Potassium has three isotopes: 39K, 40K, and 41K, but only 40K is radioactive and in most cases decays by β-decay into stable 40Ca. In potassium of natural origin, the proportion of 40K is 0.011%. The half-life of 40K is 1.25 × 109 years, and it is not hazardous to the environment [6]. 137Cs is one of the radioactive products of uranium fission in nuclear power plants and during nuclear explosions [6]. It can be harmful to human health because it is chemically similar to potassium, which means that it can act as a substitute for potassium in biochemical reactions in the human body. Moreover, its half-life is 30 years, which means that it has negative effects on the environment and living organisms for many years.
The aim of this study was to investigate how the physical and chemical composition of soil affected the soil concentration of radionuclides 238U, 40K, and 137Cs, which was based on the measured radionuclide concentrations and values of selected soil parameters in the municipality of Dvor. Additionally, ambient equivalent dose rate (H*(10)/t) was measured and annual effective dose calculated for the average person living in the area of interest. The soil surrounding the storage site acts as a natural barrier that prevents the spread of radionuclides into the environment, which makes its characterisation essential. By understanding the soil’s physical and chemical properties in relation to radionuclides, one can predict migration patterns and the potential environmental impact of radionuclides.
It is important to note that the investigated area was affected by a war about 30 years ago and is now sparsely populated, without any significant industry, and with about 40% of the area (in 2022, 1400 ha out of the total 3464 ha) used for organic farming [7]. Hence, the soil samples were all sampled from undisturbed soil in the area without human activity.
2. Materials and Methods
2.1. Soil Sampling and Measurements of H*(10)/t on Site
Soil sampling was conducted from 14 October 2020 to 29 April 2021, with the number of collected samples being 61 (roughly 1 sample per 10 km2). Sampling sites were selected from each of the 4 geological areas (L1, L2, L3, and L4), so that 15 locations were in each of L1–L3 and 16 locations were in L4 (Table 1). Sampling was carried out in accordance with the procedure for taking soil samples for studying environmental pollutants [8]. Soil was sampled from the surface to a depth of 15 cm at three (triangular scheme) or five points (cross scheme), which were ten metres apart depending on the sampling point. In the field, subsamples weighing 1.5 to 2 kg were homogenised, and 1.5 to 3 kg of the final composite sample was processed further. It should be noted that all of the samples originated from uncultivated areas, i.e., the locations of the soil samples were valleys, pastures, and meadows, often along rivers or streams. Seven samples represented soil from the forest area, where the sampling was carried out along a road surrounded by the forest.
Additionally, at each soil sampling location, we measured ambient equivalent dose rate (H*(10)/t) using a Thermo Eberline FH-40G dose rate metre (Thermo Fisher Scientific, Waltham, MA, USA). The measurements were carried out 1 m above the ground for 10 min. The average dose rate during the exposure period was used for calculating the annual external effective dose (from soil) for the average person living in the area of interest. Equation (1) was used with an outdoor occupancy of 2000 h per year. The soil sampling and dose rate measurement locations are shown in Figure 1.
D (mSv/year) = H*(10)/t (nSv/h) ∙ 2000 (h) ∙ 10−6
2.2. Laboratory Analysis
The soil samples were sieved (maximum grain size of 2 mm), dried at 105 °C for 3 days, and ashed at 400 °C. The samples were packed in sealed cylindrical containers of 200 mL according to standardised procedures [8]. Gamma-ray spectrometry measurements of the samples were carried out using the detector system of a high-purity germanium coaxial photon detector (Ortec GMX, Oak Ridge, TN, USA) with a relative efficiency of 74.2% and a full photo peak width at half maximum of 2.24 keV, both at 1.33 MeV 60Co. Energy and efficiency calibrations were performed with certified calibration sources (CBSS2 MIX in a 200 mL geometry containing 241Am, 109Cd, 139Ce, 57Co, 137Cs, 133Ba, 85Sr, 88Y, 51Cr in a silicon resin, Eurostandard CZ, Czech Republic). The measurement time was at least 80,000 s, depending on the activity of a sample, and spectra were analysed using the ORTEC Gamma Vision software (Gamma Vision 32, ORTEC/AMETEK, Oak Ridge, TN, USA). The gamma-ray spectrometry system was appropriately validated (trueness, precision/repeatability, limit of detection, matrix variation, and measurement uncertainty) [10,11]. The laboratory is accredited according to ISO/IEC 17025:2017 requirements [12]. The detection limits for 238U, 40K, and 137Cs were typically 2 Bq/kg, 4 Bq/kg, and 0.4 Bq/kg, respectively. The measurement uncertainty budget comprised emission probability, a self-attenuation correction, coincidence correction, detector efficiency, sample mass, and counting rate (background radiation subtracted).
The following soil parameters were analysed: pH, plant available phosphorus (AP), plant available potassium (AK), soil mechanical composition, carbonate content (CaCO3), hydrolytic acidity (HA), total carbon (TC), total hydrogen (TH), total nitrogen (TN), total sulphur (TS), organic matter (OM), total inorganic carbon (TIC), total organic carbon (TOC), and the content of 22 total elements (essential and non-essential). All of the methods used for physico-chemical parameters are listed in Appendix A (Table A1).
2.3. Statistical and Spatial Data Processing
The statistical analysis was carried out using the Statistica 12.64 (StatSoft, Hamburg, Germany) software and Microsoft Office Excel 2016 (Microsoft, Redmont, WA, USA). The standard deviation of the value distribution was calculated and adopted as a measure of sample variability, which is appropriate. The sampling points were spatially located using GPS coordinates and entered into the database to create a GIS map for each analysed parameter individually. The map was then used to create spatial maps in QGIS software V.3.16.8 (QGIS, Grüt (Gossau ZH), Switzerland), using the inverse distance weighted interpolation (IDW) method.
3. Results and Discussion
3.1. Radionuclide Concentration
Activity concentrations of radionuclides with their uncertainties are shown in Appendix A (Table A2). Table 2 presents the descriptive statistics of the measurement results according to the geological areas of interest, as well as mean values and ranges of values at all 61 locations.
The activity concentration of 238U in the soil ranged from 9 to 72 Bq/kg, with an average value of 54 Bq/kg. The average value for Croatia is 45 Bq/kg [13], which is similar to the value in this work. Factors such as soil type, geology, and climate influence the activity concentrations of natural radionuclides in soil. In studies like one from Ogun State, Nigeria, the estimated average values for 238U were 45 ± 10 Bq/kg. It was observed that the activity concentration of 238U ranged between 32 ± 8 and 78 ± 14 Bq/kg [14]. A study from Izmir–Ankara Highway, Turkey, determined ranges of 238U activity in the soil to be from 42.60 to 47.30 Bq/kg [15]. Another study from the same country but in a different location (Kirkareli, Turkey) suggests that the 238U activity concentration ranges from 6 to 73 Bq/kg [16].
The activity concentrations of 40K showed a large difference between the minimum and maximum concentrations, from 65 Bq/kg (L2T-11) to 823 Bq/kg (L4T-05), whereas the mean value was 531 Bq/kg. The standard deviation of the values of the 40K activity concentrations in soil was extremely high, which was expected due to the different geological properties of soils. Šoštarić et al. [17] found that 40K activity concentrations in the Dvor area were between 325 and 494 Bq/kg, and these values were within the range of activity concentrations measured in this study. The mean value for Croatia is 423 Bq/kg [13], while the mean value in the investigated area was slightly higher (531 Bq/kg), but still close to other values in Croatia [4]. For comparison, in Bangladesh 40K ranged from 279.02 to 647.82 Bq/kg, with an average of 451.90 ± 24.89 Bq/kg [17]. Activity concentrations have been observed to be spread over the range of 155–543 Bq/kg for 40K in Jordanian soil samples [18]. The range of values of the 40K activity concentrations of Istanbul soil was 294–612 Bq/kg, with an average value of 449 ± 9 Bq/kg [19].
137Cs is an anthropogenic radionuclide that was released into the environment as a result of nuclear weapons testing in the 1950s and 1960s and accidents in nuclear power plants.
Activity concentrations of 137Cs in the area of the municipality of Dvor ranged from 4 Bq/kg to 80 Bq/kg, and the mean value was 39 Bq/kg. The lowest activity concentration in the area of the municipality of Dvor measured by Šoštarić et al. [16] was 3 Bq/kg and the highest was 205 Bq/kg, which is significantly higher than the value determined in this investigation. The mean value of 137Cs in the Republic of Croatia is 25.4 Bq/kg and is slightly lower than the mean value of the area investigated here (38 Bq/kg). By looking at other studies, we can clearly see that the range of results is very similar, but in some countries, there are regions and parts with higher activity concentrations of this manmade radionuclide. For example, 137Cs was found in all samples from Bangladesh to have an average of 2.41 ± 0.18 Bq/kg and to range from 0.18 to 5.07 Bq/kg [18]. The average value of 137Cs in Kirkareli, Turkey, was 8 ± 5 Bq/kg [20]. The typical concentration of 137Cs found in topsoils in Jordan ranged from 7.5 to 576 Bq/kg [18]. The activity concentrations of 137Cs in soils from a Bulgaria–Turkey border region were found to range from 1.71 ± 0.18 Bq/kg to 6.99 ± 0.66 Bq/kg [21].
All of the results from other studies are below global average values for natural radionuclides (35 and 400 Bq/kg for 238U and 40K, respectively) reported by the United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) [22].
3.2. Spatial Distribution of Radionuclides
Spatial distribution maps are a good tool to show adequate information on measurement results visually and are usually needed by regulatory authorities for identifying potentially contaminated areas. Figure 2 presents spatial distribution maps for 238U, 40K, 137Cs, and H*(10)/t in the investigated area of Dvor municipality.
As seen in Figure 2, spatial distributions depend on the geology of the area. Although the range of values was not large, there were some hotspots. The activity concentrations of 238U were higher in the L3 area (Cenozoic area and associated Quaternary deposits along watercourses), which is similar to the H*(10)/t map values. On the northern side of the L4 area, there was an obvious hotspot in 137Cs activity concentration levels, which also agreed with the dose rate results.
3.3. Ambient Equivalent Dose Rate
The results of ambient equivalent dose rate (H*(10)/t) measurements are shown in Table 3 together with the parameters of their descriptive statistics. Detailed data are shown in Appendix A, Table A3. The values ranged from 52 nSv/h (L2T-10) to 130 nSv/h (L1T-03, L3T-03). These values are in agreement with the average ambient equivalent dose rate in Croatia [17], and there was a general trend where certain geological formations correlated with higher or lower radiation levels. Locations on Palaeozoic formations had moderate radiation levels (86–94 nSv/h). This suggests slightly elevated natural background radiation in these areas. Cenozoic areas showed moderate radiation levels (86 nSv/h) similar to Palaeozoic locations. However, L3T-15 (Cenozoic/Mesozoic border) had a much higher value, indicating possible geological influences at the transition zone. The alluvia of the Una (L2T-01) and the Žirovnica (L2T-12) rivers showed lower radiation values (58–91 nSv/h), confirming that alluvial deposits generally have lower radiation levels.
3.4. Physico-Chemical Parameters
Table 4 shows a detailed comparison of average values in the areas of interest (L1–L4) and the minimum, maximum, and mean values of the physico-chemical parameters.
Table 5 shows the average values of the studied elements according to the areas of interest (L1–L4) and the total minimum, maximum, and mean values, expressed in mg/kg.
3.5. The Correlation Matrix
The correlation matrix is shown in Appendix A, Table A4, and gives a detailed visualisation of the correlations between variables in this study.
238U showed a significant positive moderate correlation with thorium (r = 0.48) and titanium (r = 0.45), as well as positive strong correlations with hydrolytic acidity (r = 0.57), aluminium concentration (r = 0.61), silicon (r = 0.70), potassium (r = 0.61), rubidium (r = 0.70), zirconium (r = 0.70), niobium (r = 0.66), and yttrium (r = 0.64). 238U was weakly positively correlated with sand content (r = 0.32), iron concentration (r = 0.31), and tungsten (r = 0.40). 238U was strongly negatively correlated with pH (r = −0.63), silt content (r = −0.55), CaCO3 (r = −0.67), calcium (r = −0.69), total carbon (r = −0.64), and total inorganic carbon (r = −0.67), and negatively weakly correlated with plant available P (r = −0.33), strontium (r = −0.34), organic matter (r = −0.28), and organic carbon (r = −0.28).
40K was strongly positively correlated with rubidium (r = 0.66) and yttrium (r = 0.51). Potassium showed moderate positive correlations with aluminium (r = 0.50), silicon (r = 0.46), iron (r = 0.42), and zinc (r = 0.43), and weak correlations with hydrolytic acidity (r = 0.30), titanium (r = 0.30), zirconium (r = 0.35), niobium (r = 0.39), phosphorus (r = 0.26), thorium (r = 0.26), total hydrogen (r = 0.30), and total nitrogen (r = 0.29).
137Cs showed only a weak correlation with particle size, namely sand composition, Si and TN.
Soil pH significantly influences the behaviour and mobility of radionuclides in the environment. In alkaline soils (high pH), radionuclides tend to form insoluble precipitates such as carbonates and hydroxides, which reduce their availability and mobility. However, in acidic soils (low pH), increased concentrations of hydrogen ions can displace radionuclide cations, enhancing their mobility [23,24].
4. Conclusions
A comprehensive physico-chemical and radionuclide characterisation of the soil near a future radioactive waste storage facility is fundamental to thoroughly assessing its long-term suitability and ensuring the continued environmental safety of the surrounding area. The results of this study are of crucial importance for evaluating the soil quality in the area of the municipality of Dvor. The correlation between the physico-chemical properties of the soil and the concentration of selected radionuclides was established. Most of the determined soil parameters showed a moderate (Th, Ti), strong (HA, Al, Si, K, Rb, Zr, Nb, Y, pH, silt content, CaCO3, Ca, TC, TIC), or weak (sand content, Fe, W, AP, Sr, OM, TOC) correlation with the radionuclide 238U. The correlations with 40K were strong (Rb, Y, CaCO3, Ca, TIC), moderate (Al, Si, Fe, Zn, silt content, TC), or weak (HA, Ti, Zr, Nb, P, Th, TH, TN, pH), and the smallest number of soil parameters, namely three, showed a positive weak correlation (sand content, Si, TN) with 137Cs concentrations in the soil. Geological formations are characterised by different radiation levels. Older formations (Palaeozoic, Cenozoic/Mesozoic border) tended to have higher radiation. Younger formations (Alluvium of the Una and Žirovnica rivers) exhibited lower radiation levels. At certain locations, the average background radiation was exceeded. Ambient dose rates varied across the study area, with higher values observed in certain geological formations (e.g., Palaeozoic and the Cenozoic/Mesozoic border), potentially due to elevated natural background radiation from higher uranium or thorium content in those formations. Alluvial deposits generally showed lower dose rates.
The data obtained in this study can be used as reference data for monitoring possible radioactive pollution in the future or for radioactivity mapping of the studied area. It can be concluded that the results suggest only a potential relationship between physico-chemical soil characteristics and radionuclide concentrations. More detailed investigation with time-repeated analyses or detailed geological/transport models are needed to obtain firm evidence of the relationship. Overall, the findings highlight the importance of considering geological heterogeneity and the correlation between soil properties and radionuclide distribution when assessing the suitability of a site for radioactive waste storage. An understanding of the physical and chemical properties of soil helps identify possible hotspots for a future monitoring programme. Additionally, these kinds of characterisations enable the development of robust containment strategies and inform the necessary intervention services, which should ensure the long-term security of radioactive waste storage sites. Through detailed and systematic assessments, it is possible to enhance regulatory frameworks and improve the design of facilities for safe and efficient waste management.
Author Contributions
T.B.: writing, sampling, data analysis, reviewing and editing, B.P.: writing, analysis of the results, correspondence; M.N.: writing, methodology, analysis writing; D.B.: radionuclide analyses, reviewing; D.R.: radionuclide analyses, reviewing; I.H.: spatial distribution analyses, GIS; M.G.: soil physico-chemical analyses, writing, reviewing; A.P.: conceptualisation and study design, reviewing; I.Š.: sampling, soil physico-chemical analyses; I.K.: reviewing; A.R.: conceptualisation and study design, reviewing; Ž.Z.: conceptualisation, writing, analysis of the results, reviewing. All authors have read and agreed to the published version of the manuscript.
Funding
This investigation was funded by a fund for financing the decommissioning of the Krško Nuclear Power Plant and the disposal of Krško NPP radioactive waste and spent nuclear fuel. Additionally, this work was partly funded by the Division of Radiation Protection of the Institute for Medical Research and Occupational Health and the European Union—Next Generation EU (Program Contract of 8 December 2023, Class: 643-02/23-01/00016, Reg. no. 533-03-23-0006; EBDIZ). Part of the research was performed using the facilities and equipment funded by the European Regional Development Fund project KK.01.1.1.02.0007, “Research and Education Centre of Environmental Health and Radiation Protection—Reconstruction and Expansion of the Institute for Medical Research and Occupational Health”.
Data Availability Statement
Data used in this investigation are publicly partly available within the report for measurement of radioactivity to define the baseline (existing) state at the site of the radioactive waste management centre and in the municipality of Dvor with an individual dose assessment (available from https://www.fond-nek.hr/en/ (accessed on 15 December 2024)). Physico-chemical soil analysis was carried out within the diploma thesis “Determination of Natural and Anthropogenic Radionuclides in the Soil of Dvor Municipality” by MS Agroecology student Martina Novosel.
Acknowledgments
The authors would like to thank all of the staff of the Division of Radiation Protection of the Institute for Medical Research and Occupational Health in Zagreb who participated in sampling and analysis of the results.
Conflicts of Interest
The authors declare that there are no conflicts of interest.
Appendix A
Table A1.
Soil physico-chemical parameters and methods used, followed by the specific protocol (standard).
Table A1.
Soil physico-chemical parameters and methods used, followed by the specific protocol (standard).
| Parameter | Unit | Method | Protocol/Standard |
|---|---|---|---|
| Drying/grinding/ seeding/homogenisation | - | Preparation of soil samples | ISO 11464:2006 [25] |
| pH | - | Determination of the pH value in 0.01 M CaCl2, 1 M KCl, and H2O in a ratio of 1:2.5 (m/v) | ISO 10390:2005 [26] |
| Hydrolytic acidity (HA) | cmol+/kg | Extraction with 1M NaAc | Škorić 1982 [27] |
| Plant available phosphorus (AP) and potassium (AK) | mg/100 g | In AL extract in a ratio of 1:20 (m/v) AL method (spectrophotometer, Hach DR/2000, 1996; and flame photometer, Jenway, PFP7, 1999) | Škorić 1982 [27] |
| Mechanical composition of the soil (sand, silt, clay) | % | Sieving and sedimentation Soil quality—determination of particle size distribution in mineral soil material—method by sieving and sedimentation | ISO 11277:2020 [28] |
| Total elements (As, Cr, Pb, Al, Si, Fe, Ca, Ti, K, Mn, Rb, Zr, Nb, Ni, P, Y, Zn, Sr, Th, Cu., W, Co) | mg/kg | Soil quality—screening soils for selected elements by energy-dispersive X-ray fluorescence spectrometry using a handheld or portable instrument (pXRF Vanta, Olympus, 2019) | ISO 13196:2013 [29] |
| Organic matter (OM), TOC and TC | % | Dry combustion method, Vario Macro CHNS (TC) | ISO 10694:2021 [30] |
| TN | % | Soil quality—determination of total nitrogen content by dry combustion (“elemental analysis”) | ISO 13878:2020 [31] |
| TS | % | Soil quality—determination of total sulphur content by dry combustion | ISO 15178:2021 [32] |
| CaCO3 | % | Volumetric method (Scheibler) (TIC) | ISO 10693:2004 [33] |
Table A2.
Activity concentrations of radionuclides (238U, 40K, 137Cs) in Bq/kg.
| Sample ID | 238U | 40K | 137Cs | Sample ID | 238U | 40K | 137Cs |
|---|---|---|---|---|---|---|---|
| A ± U * [Bq/kg] | A ± U * [Bq/kg] | ||||||
| L1T-01 | 42.7 ± 0.7 | 283 ± 1 | 51.5 ± 0.2 | L3T-01 | 55.7 ± 0.9 | 661 ± 2 | 53.4 ± 0.2 |
| L1T-02 | 62.3 ± 0.9 | 515 ± 2 | 48.4 ± 0.2 | L3T-02 | 47.1 ± 0.8 | 499 ± 2 | 26.2 ± 0.1 |
| L1T-03 | 43.6 ± 0.7 | 328 ± 1 | 38.6 ± 0.1 | L3T-03 | 54.3 ± 0.9 | 501 ± 2 | 30.1 ± 0.1 |
| L1T-04 | 65.1 ± 1.0 | 553 ± 2 | 50.4 ± 0.2 | L3T-04 | 38.7 ± 0.7 | 517 ± 2 | 40.3 ± 0.1 |
| L1T-05 | 44.5 ± 0.8 | 470 ± 2 | 56.1 ± 0.2 | L3T-05 | 50.6 ± 0.9 | 512 ± 2 | 38.3 ± 0.1 |
| L1T-06 | 54.3 ± 0.9 | 548 ± 2 | 29.9 ± 0.1 | L3T-06 | 42.8 ± 0.7 | 524 ± 2 | 7.07 ± 0.06 |
| L1T-07 | 61 ± 1 | 596 ± 2 | 33.5 ± 0.1 | L3T-07 | 51.7 ± 0.6 | 351 ± 1 | 79.7 ± 0.2 |
| L1T-08 | 50.5 ± 0.8 | 415 ± 2 | 36.2 ± 0.1 | L3T-08 | 57.6 ± 0.9 | 412 ± 2 | 27.9 ± 0.1 |
| L1T-09 | 66.8 ± 0.9 | 664 ± 2 | 42.5 ± 0.1 | L3T-09 | 61.3 ± 0.9 | 503 ± 2 | 44.4 ± 0.1 |
| L1T-10 | 61.6 ± 0.9 | 617 ± 2 | 34.67 ± 0.01 | L3T-10 | 51.1 ± 0.9 | 496 ± 3 | 67.4 ± 0.1 |
| L1T-11 | 57.7 ± 0.9 | 487 ± 2 | 58.4 ± 0.2 | L3T-11 | 55.1 ± 0.9 | 556 ± 2 | 28.6 ± 0.1 |
| L1T-12 | 66.6 ± 0.9 | 530 ± 2 | 49.9 ± 0.1 | L3T-12 | 42 ± 2 | 493 ± 2 | 29.8 ± 0.1 |
| L1T-13 | 60.7 ± 0.7 | 575 ± 2 | 30.5 ± 0.1 | L3T-13 | 49.1 ± 0.9 | 573 ± 2 | 49.4 ± 0.2 |
| L1T-14 | 66.7 ± 0.7 | 571 ± 19 | 32.9 ± 0.1 | L3T-14 | 54.5 ± 0.9 | 485 ± 2 | 43.4 ± 0.1 |
| L1T-15 | 59.4 ± 0.8 | 606 ± 2 | 17.2 ± 0.1 | L3T-15 | 50.1 ± 0.1 | 523 ± 2 | 77.6 ± 0.2 |
| L2T-01 | 34.7 ± 0.7 | 372 ± 2 | 36.1 ± 0.1 | L4T-01 | 65.2 ± 0.9 | 592 ± 2 | 14.8 ± 0.1 |
| L2T-02 | 41.6 ± 0.7 | 398 ± 1 | 59.5 ± 0.2 | L4T-02 | 48.3 ± 0.8 | 529 ± 2 | 28.1 ± 0.1 |
| L2T-03 | 48.1 ± 0.8 | 503 ± 2 | 51.1 ± 0.2 | L4T-03 | 43.5 ± 0.8 | 502 ± 2 | 19.9 ± 0.1 |
| L2T-04 | 40.5 ± 0.8 | 515 ± 2 | 43.9 ± 0.1 | L4T-04 | 69.8 ± 0.9 | 592 ± 2 | 15.4 ± 0.1 |
| L2T-05 | 55.2 ± 0.9 | 650 ± 2 | 38.1 ± 0.1 | L4T-05 | 68 ± 1 | 823 ± 2 | 39.7 ± 0.1 |
| L2T-06 | 51.2 ± 0.9 | 654 ± 2 | 41.4 ± 0.1 | L4T-06 | 66 ± 1 | 706 ± 2 | 50.5 ± 0.2 |
| L2T-07 | 60 ± 1 | 626 ± 2 | 31.7 ± 0.1 | L4T-07 | 49.6 ± 0.9 | 498 ± 2 | 23.6 ± 0.1 |
| L2T-08 | 33.2 ± 0.7 | 311 ± 1 | 26.6 ± 0.1 | L4T-08 | 54.9 ± 0.9 | 556 ± 2 | 31.3 ± 0.1 |
| L2T-09 | 58.5 ± 0.9 | 537 ± 2 | 25.3 ± 0.1 | L4T-09 | 64 ± 1 | 617 ± 2 | 26.0 ± 0.1 |
| L2T-10 | 9.0 ± 0.6 | 65 ± 1 | 4.16 ± 0.05 | L4T-10 | 59.4 ± 0.9 | 586 ± 2 | 54.7 ± 0.2 |
| L2T-11 | 54.7 ± 0.8 | 512 ± 2 | 23.8 ± 0.1 | L4T-11 | 43.7 ± 0.8 | 487 ± 2 | 40.9 ± 0.1 |
| L2T-12 | 60.7 ± 0.9 | 549 ± 2 | 33.3 ± 0.1 | L4T-12 | 69 ± 1 | 599 ± 2 | 61.2 ± 0.2 |
| L2T-13 | 52.8 ± 0.8 | 589 ± 2 | 35.3 ± 0.1 | L4T-13 | 72 ± 1 | 640 ± 2 | 44.9 ± 0.1 |
| L2T-14 | 53.8 ± 0.9 | 569 ± 2 | 49.8 ± 0.2 | L4T-14 | 47.7 ± 0.9 | 604 ± 2 | 68.2 ± 0.2 |
| L2T-15 | 51.7 ± 0.8 | 633 ± 2 | 45.9 ± 0.1 | L4T-15 | 60.3 ± 0.9 | 635 ± 2 | 33.0 ± 0.1 |
| L4T-16 | 57.4 ± 0.9 | 574 ± 2 | 7.68 ± 0.07 | ||||
* A-activity concentration in Bq/kg; U-expended measurement uncertainty in Bq/kg.
Table A3.
Ambient dose equivalent rate (nSv/h) and yearly effective dose (nSv/year) measured at 61 locations.
Table A3.
Ambient dose equivalent rate (nSv/h) and yearly effective dose (nSv/year) measured at 61 locations.
| Location | H*(10)/t ± U * (nSv/h) | Effective Dose (mSv/year) | Location | H*(10)/t ± U * (nSv/h) | Effective Dose (mSv/year) |
|---|---|---|---|---|---|
| L1T-01 | 86 ± 30 | 0.171 | L3T-01 | 86 ± 30 | 0.171 |
| L1T-02 | 76 ± 27 | 0.153 | L3T-02 | 76 ± 27 | 0.153 |
| L1T-03 | 130 ± 46 | 0.260 | L3T-03 | 130 ± 46 | 0.260 |
| L1T-04 | 72 ± 25 | 0.145 | L3T-04 | 72 ± 25 | 0.145 |
| L1T-05 | 76 ± 27 | 0.152 | L3T-05 | 76 ± 27 | 0.152 |
| L1T-06 | 99 ± 35 | 0.198 | L3T-06 | 99 ± 35 | 0.198 |
| L1T-07 | 82 ± 29 | 0.164 | L3T-07 | 82 ± 29 | 0.164 |
| L1T-08 | 74 ± 26 | 0.148 | L3T-08 | 74 ± 26 | 0.148 |
| L1T-09 | 118 ± 41 | 0.236 | L3T-09 | 118 ± 41 | 0.236 |
| L1T-10 | 87 ± 30 | 0.174 | L3T-10 | 87 ± 30 | 0.174 |
| L1T-11 | 112 ± 39 | 0.223 | L3T-11 | 112 ± 39 | 0.223 |
| L1T-12 | 94 ± 33 | 0.188 | L3T-12 | 94 ± 33 | 0.188 |
| L1T-13 | 95 ± 33 | 0.189 | L3T-13 | 95 ± 33 | 0.189 |
| L1T-14 | 80 ± 28 | 0.159 | L3T-14 | 80 ± 28 | 0.159 |
| L1T-15 | 117 ± 41 | 0.234 | L3T-15 | 117 ± 41 | 0.234 |
| L2T-01 | 58 ± 20 | 0.116 | L4T-01 | 94 ± 33 | 0.188 |
| L2T-02 | 103 ± 36 | 0.206 | L4T-02 | 60 ± 21 | 0.120 |
| L2T-03 | 90 ± 32 | 0.181 | L4T-03 | 59 ± 21 | 0.118 |
| L2T-04 | 82 ± 29 | 0.164 | L4T-04 | 90 ± 32 | 0.180 |
| L2T-05 | 80 ± 28 | 0.160 | L4T-05 | 106 ± 37 | 0.212 |
| L2T-06 | 82 ± 29 | 0.165 | L4T-06 | 115 ± 40 | 0.230 |
| L2T-07 | 74 ± 26 | 0.147 | L4T-07 | 91 ± 32 | 0.182 |
| L2T-08 | 95 ± 33 | 0.190 | L4T-08 | 95 ± 33 | 0.190 |
| L2T-09 | 87 ± 31 | 0.175 | L4T-09 | 110 ± 39 | 0.220 |
| L2T-10 | 52 ± 18 | 0.104 | L4T-10 | 97 ± 34 | 0.193 |
| L2T-11 | 91 ± 32 | 0.182 | L4T-11 | 86 ± 30 | 0.172 |
| L2T-12 | 91 ± 32 | 0.182 | L4T-12 | 113 ± 40 | 0.226 |
| L2T-13 | 73 ± 26 | 0.146 | L4T-13 | 124 ± 43 | 0.248 |
| L2T-14 | 75 ± 26 | 0.149 | L4T-14 | 70 ± 25 | 0.140 |
| L2T-15 | 86 ± 30 | 0.172 | L4T-15 | 81 ± 28 | 0.162 |
| L4T-16 | 92 ± 32 | 0.185 |
* U-expended measurement uncertainty (nSv/h).
Table A4.
Correlation matrix of determined radionuclides and physico-chemical soil properties (red marked correlations are significant at p < 0.05).
Table A4.
Correlation matrix of determined radionuclides and physico-chemical soil properties (red marked correlations are significant at p < 0.05).
| pH | AP | AK | Sand | Silt | Clay | As | Cr | Pb | U238 | |
| U238 | −0.63 | −0.33 | −0.02 | −0.55 | 0.32 | 0.19 | 0.21 | −0.22 | 0.08 | 1.00 |
| K40 | −0.35 | −0.03 | 0.14 | −0.43 | 0.17 | 0.24 | 0.18 | 0.04 | 0.09 | 0.76 |
| Cs137 | 0.17 | 0.12 | 0.12 | −0.16 | 0.27 | −0.14 | 0.17 | 0.20 | −0.06 | 0.08 |
| K40 | Cs137 | CaCO3 | HA | Al | Si | Fe | Ca | Ti | K | |
| U238 | 0.76 | 0.08 | −0.67 | 0.57 | 0.61 | 0.70 | 0.31 | −0.69 | 0.45 | 0.61 |
| K40 | 1.00 | 0.01 | −0.62 | 0.30 | 0.50 | 0.46 | 0.42 | −0.63 | 0.30 | 0.64 |
| Cs137 | 0.01 | 1.00 | −0.20 | −0.15 | −0.11 | 0.26 | −0.10 | −0.20 | 0.04 | 0.00 |
| Mn | Rb | Zr | Nb | Ni | P | Y | Zn | Sr | Th | |
| U238 | 0.18 | 0.70 | 0.70 | 0.66 | −0.15 | −0.05 | 0.64 | 0.13 | −0.34 | 0.48 |
| K40 | 0.12 | 0.66 | 0.35 | 0.39 | 0.17 | 0.26 | 0.51 | 0.43 | −0.12 | 0.26 |
| Cs137 | 0.02 | 0.03 | 0.22 | 0.00 | 0.10 | 0.03 | 0.04 | 0.02 | 0.02 | 0.02 |
| Cu | W | Co | TC | TH | TN | TS | OM | TIC | TOC | |
| U238 | −0.09 | 0.40 | 0.20 | −0.64 | 0.09 | −0.04 | −0.02 | −0.28 | −0.67 | −0.28 |
| K40 | 0.25 | 0.20 | 0.22 | −0.46 | 0.30 | 0.29 | 0.24 | −0.03 | −0.62 | −0.03 |
| Cs137 | 0.04 | −0.05 | 0.05 | −0.04 | 0.14 | 0.28 | 0.22 | 0.20 | −0.20 | 0.20 |
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Figure 1.
(a) Locations of soil sampling and ambient equivalent dose rate measurements (61 locations—red circles). The location of the future radioactive waste storage site is marked with a black circle. (b) Geological areas (L1—surroundings of the waste management centre with Palaeozoic (Pz), Triassic, and associated alluvial or Quaternary (Q) deposits; L2—alluvial deposits of the Una and the Žirovnica rivers; L3—Cenozoic area and associated Quaternary deposits along watercourses; L4—Palaeozoic or Mesozoic (Mz) area and associated Quaternary deposits along watercourses). The location of the future radioactive waste storage site is marked with a blue star (map reference [9]).
Figure 1.
(a) Locations of soil sampling and ambient equivalent dose rate measurements (61 locations—red circles). The location of the future radioactive waste storage site is marked with a black circle. (b) Geological areas (L1—surroundings of the waste management centre with Palaeozoic (Pz), Triassic, and associated alluvial or Quaternary (Q) deposits; L2—alluvial deposits of the Una and the Žirovnica rivers; L3—Cenozoic area and associated Quaternary deposits along watercourses; L4—Palaeozoic or Mesozoic (Mz) area and associated Quaternary deposits along watercourses). The location of the future radioactive waste storage site is marked with a blue star (map reference [9]).
Figure 2.
Spatial distribution of 238U, 40K, 137Cs, and H*(10)/t in the area of interest.
Table 1.
Geological areas of sampling and sample IDs.
| Area (Sample ID) | Geological Description | Number of Sampling Points |
|---|---|---|
| L1 (L1T-01–L1T-15) | Surroundings of the waste management centre- Palaeozoic (Pz), Triassic, and associated alluvial or Quaternary (Q) deposits | n = 15 |
| L2 (L2T-01–L2T-15) | Alluvial deposits of the Una and Žirovnica rivers | n = 15 |
| L3 (L2T-01–L2T-15) | Cenozoic area and associated Quaternary deposits along watercourses | n = 15 |
| L4 (L2T-01–L2T-16) | Palaeozoic or Mesozoic (Mz) area and associated Quaternary deposits along watercourses | n = 16 |
Table 2.
Activity concentrations of radionuclides (238U, 40K, 137Cs) in Bq/kg (mean and standard deviation for each geological area, and mean values and range for all 61 locations; n = number of samples).
Table 2.
Activity concentrations of radionuclides (238U, 40K, 137Cs) in Bq/kg (mean and standard deviation for each geological area, and mean values and range for all 61 locations; n = number of samples).
| 238U [Bq/kg] | 40K [Bq/kg] | 137Cs [Bq/kg] | ||||
|---|---|---|---|---|---|---|
| Mean | SD | Mean | SD | Mean | SD | |
| L1 (n = 15) | 58 | 9 | 517 | 106 | 40 | 12 |
| L2 (n = 15) | 47 | 14 | 499 | 158 | 36 | 14 |
| L3 (n = 15) | 51 | 6 | 507 | 68 | 43 | 20 |
| L4 (n = 16) | 59 | 10 | 596 | 83 | 35 | 18 |
| Mean (n = 61) | 54 | 531 | 39 | |||
| Range (n = 61) | 9–72 | 65–823 | 4–80 | |||
Table 3.
Ambient equivalent dose rate (H*(10)/t) (mean and standard deviation for each geological area, and mean values and range for all 61 locations).
Table 3.
Ambient equivalent dose rate (H*(10)/t) (mean and standard deviation for each geological area, and mean values and range for all 61 locations).
| H*(10)/t Mean ± SD [nSv/h] | Effective Dose (mSv/year) | |
|---|---|---|
| L1 (n = 15) | 93 ± 18 | 0.186 ± 0.04 |
| L2 (n = 15) | 81 ± 13 | 0.162 ± 0.03 |
| L3 (n = 15) | 93 ± 18 | 0.186 ± 0.04 |
| L4 (n = 16) | 93 ± 19 | 0.185 ± 0.04 |
| Mean (n = 61) | 90 | 0.180 |
| Range (n = 61) | 52–130 | 0.104–0.260 |
Table 4.
Soil physico-chemical parameters.
| pH | Mechanical Composition of the Soil | AP * (mg P2O5 /100 g of Soil) | AK * (mg K2O/100 g of Soil) | CaCO3 * (%) | HA * (cmol+/kg) | |||
| Sand (%) | Silt (%) | Clay (%) | ||||||
| L1 (n = 15) | 5.46 | 22 | 49 | 28 | 1.7 | 6.8 | 0.51 | 12.9 |
| L2 (n = 15) | 6.97 | 21 | 57 | 23 | 8.1 | 9.6 | 9.71 | 3.3 |
| L3 (n = 15) | 6.18 | 18 | 53 | 29 | 7.0 | 16.9 | 1.41 | 7.2 |
| L4 (n = 16) | 5.55 | 21 | 49 | 30 | 4.0 | 14.2 | 0.38 | 14.1 |
| Mean (n = 61) | 6.03 | 20 | 52 | 28 | 5.2 | 11.9 | 2.96 | 9.5 |
| Min (n = 61) | 4.15 | 2 | 10 | 2 | 0.3 | 1.3 | 0.01 | 0.1 |
| Max (n = 61) | 8.52 | 88 | 78 | 61 | 34.3 | 92.1 | 76.2 | 26.6 |
| TC * (%) | TH * (%) | TN * (%) | TS * (%) | TIC * (%) | TOC * (%) | OM * (%) | ||
| L1 (n = 15) | 2.5 | 1.085 | 0.207 | 0.047 | 0.06 | 2.4 | 4.1 | |
| L2 (n = 15) | 4.3 | 1.245 | 0.267 | 0.055 | 1.16 | 3.1 | 5.4 | |
| L3 (n = 15) | 3.2 | 1.313 | 0.283 | 0.056 | 0.17 | 3.0 | 5.3 | |
| L4 (n = 16) | 3.6 | 1.427 | 0.314 | 0.059 | 0.05 | 3.6 | 6.2 | |
| Mean (n = 61) | 3.4 | 1.270 | 0.269 | 0.054 | 0.36 | 3.04 | 5.2 | |
| Min (n = 61) | 0.7 | 0.373 | 0.066 | 0.016 | 0.001 | 0.71 | 1.2 | |
| Max (n = 61) | 13.2 | 2.300 | 0.494 | 0.076 | 9.14 | 5.51 | 9.5 | |
* Plant available phosphorus (AP), plant available potassium (AK), carbonate content (CaCO3), hydrolytic acidity (HA), total carbon (TC), total hydrogen (TH), total nitrogen (TN), total sulphur (TS), organic matter (OM), total inorganic carbon (TIC), total organic carbon (TOC).
Table 5.
Average values of elements by area and total minimum, maximum, and mean values, expressed in mg/kg.
Table 5.
Average values of elements by area and total minimum, maximum, and mean values, expressed in mg/kg.
| As | Cr | Pb | Al | Si | Fe | Ca | Ti | |
| [mg/kg] | ||||||||
| L1 | 15 | 108 | 37 | 122,367 | 447,159 | 36,328 | 4387 | 6134 |
| L2 | 12 | 149 | 25 | 102,887 | 383,596 | 35,878 | 43,274 | 5593 |
| L3 | 12 | 168 | 21 | 103,540 | 421,877 | 35,885 | 10,041 | 6019 |
| L4 | 11 | 116 | 97 | 121,813 | 419,699 | 38,756 | 5357 | 6161 |
| Mean | 12 | 135 | 46 | 112,802 | 418,109 | 36,745 | 15,594 | 5980 |
| Min | 1 | 76 | 5 | 38,132 | 118,833 | 8087 | 1625 | 1406 |
| Max | 27 | 291 | 696 | 149,778 | 513,622 | 57,113 | 277,890 | 9467 |
| K | Mn | Rb | Zr | Nb | Ni | P | ||
| [mg/kg] | ||||||||
| L1 | 23,628 | 1009 | 117 | 309 | 20 | 29 | 157 | |
| L2 | 19,040 | 786 | 99 | 240 | 17 | 61 | 206 | |
| L3 | 19,363 | 818 | 99 | 305 | 19 | 56 | 168 | |
| L4 | 24,856 | 959 | 123 | 291 | 22 | 39 | 186 | |
| Mean | 21,773 | 894 | 110 | 286 | 20 | 46 | 179 | |
| Min | 4507 | 344 | 14 | 35 | 5 | 7 | 57 | |
| Max | 32,111 | 1602 | 162 | 414 | 29 | 135 | 519 | |
| Y | Zn | Sr | Th | Cu | W | Co | ||
| [mg/kg] | ||||||||
| L1 | 32 | 97 | 96 | 11 | 20 | 3 | 13 | |
| L2 | 30 | 99 | 121 | 8 | 25 | 2 | 11 | |
| L3 | 30 | 90 | 125 | 9 | 25 | 2 | 11 | |
| L4 | 33 | 108 | 95 | 10 | 29 | 3 | 14 | |
| Mean | 31 | 98 | 109 | 9 | 25 | 3 | 12 | |
| Min | 10 | 33 | 64 | 2 | 4 | 2 | 3 | |
| Max | 40 | 204 | 459 | 20 | 46 | 4 | 27 | |
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Bituh, T.; Petrinec, B.; Novosel, M.; Babić, D.; Rašeta, D.; Hrelja, I.; Galić, M.; Perčin, A.; Širić, I.; Kisić, I.; et al. The Physico-Chemical and Radionuclide Characterisation of Soil near a Future Radioactive Waste Management Centre. Environments 2025, 12, 121. https://doi.org/10.3390/environments12040121
AMA Style
Bituh T, Petrinec B, Novosel M, Babić D, Rašeta D, Hrelja I, Galić M, Perčin A, Širić I, Kisić I, et al. The Physico-Chemical and Radionuclide Characterisation of Soil near a Future Radioactive Waste Management Centre. Environments. 2025; 12(4):121. https://doi.org/10.3390/environments12040121
Chicago/Turabian StyleBituh, Tomislav, Branko Petrinec, Martina Novosel, Dinko Babić, Davor Rašeta, Iva Hrelja, Marija Galić, Aleksandra Perčin, Ivan Širić, Ivica Kisić, and et al. 2025. "The Physico-Chemical and Radionuclide Characterisation of Soil near a Future Radioactive Waste Management Centre" Environments 12, no. 4: 121. https://doi.org/10.3390/environments12040121
APA StyleBituh, T., Petrinec, B., Novosel, M., Babić, D., Rašeta, D., Hrelja, I., Galić, M., Perčin, A., Širić, I., Kisić, I., Rapić, A., & Zgorelec, Ž. (2025). The Physico-Chemical and Radionuclide Characterisation of Soil near a Future Radioactive Waste Management Centre. Environments, 12(4), 121. https://doi.org/10.3390/environments12040121
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