Distribution and impacts of contamination by natural and artificial radionuclides in attic dust and urban soil samples from a former industrial Hungarian city: A case study from Salgótarján.

Primordial radionuclides can be found in all environmental compartments. Since coal-fired power plants (CFPP) can be a source of additional radionuclide contamination because coal contains natural radioactive isotopes such as 238U (226Ra) and 232Th. This study investigated the impact of such possible radionuclide contamination from former heavy industrial activities, namely a former local coal-fired power plant, in urban soils and attic dust in Salgótarján, Hungary. Even today, industrial by-products, e.g., coal ash, in this city represent significant threat to its residents. A total of 36 attic dust samples (family houses, kindergartens, churches and blockhouses) were collected and 19 urban soil samples (playgrounds, kindergartens, parks and others) were selected no further than 500 m from the corresponding attic dust sampling sites. Additionally, a coal ash and a brown forest soil sample were also collected to differentiate between the anthropogenic and geogenic sources in the residential area. The sampled houses, built between 1890 and 1990, are considered to be representative sampling sites for long-term accumulations of attic dust. The mean values of the total U, Th and Cs (mg kg-1) concentrations as well as those of K (m/m %) in attic dust and urban soil samples are 2.4, 3.6, 1.7 and 0.6 and 1.1, 4.4, 1.2 and 0.3, respectively, measured using ICP-MS. The mean activity concentrations of 226Ra, 232Th, 40K and 137Cs in attic dust and urban soil samples are 43.3, 34.0, 534.4 and 88.5 and 25.1, 32.8, 386.4 and 5.6 Bq kg-1, respectively, by using a low-background iron chamber with a well-type HPGe and a n-type coaxial HPGe detector. The elemental compositions (U, Th) and activity concentrations (226Ra, 232Th) along with their abundances in coal ash from the CFPP increase in both studied media as the distance of the sampling sites from the CFPP decreases. Two outlier attic dust samples in particular show significantly high activity concentrations of 226Ra: 145 and 143, of 232Th: 83 and 94 Bq kg-1, which can be considered as a proxy of unweathered coal ash. The calculated total absorbed gamma dose rate (D) and annual effective dose (E) received from urban soils indicate that the presence of the CFPP, coal ash cone and slag dumps does not cause an increase in the level of background radiation in Salgótarján. However, the concentrations of the studied radionuclides are much higher (except for 232Th) and exhibit higher degree of variability in the samples of attic dustthan in those of urban soils. The study suggests that attic dust preserves the undisturbed 'fingerprints' of long-term atmospheric deposition thanks to its chemical and physical properties unlike urban soil.

Estimated versus field measured soil gas radon concentration and soil gas permeability.

Prediction of areas with elevated natural radiation is fundamental for the prevention of human exposure. Soil gas radon activity concentration and soil gas permeability are predictive parameters for the radon potential, which has great importance in areas where future urban development is planned. In this study, the soil gas radon equilibrium concentration (C∞) and soil gas permeability (K) were estimated through the application of theoretical and empirical models found in the literature. These models apply soil properties as input parameters. Using already existing soil parameters to predict the radon potential of an area would be useful in avoiding direct field measurements. Therefore, in this study, we examined whether the estimated soil gas radon activity concentration and soil gas permeability values match the values measured in the field. The soil gas radon activity concentration estimated by two theoretical models is about 50% of the measured value in the studied area. This underestimation can be attributed to the assumption that the radon activity concentration measured in the field depends only on soil parameters and the models do not take into account the underlying bedrock. Additionally, these models neglect the radon transport by advection and consider only the radon availability and migration in homogeneous media. Furthermore, they do not count certain characteristics of the soil that can be relevant, e.g. organic matter and clay content in the soil. To investigate more in detail such soil characteristics, seven samples located roughly along the slope, were selected to determine the soil chemical composition by ICP-MS. Evaluating the physical and chemical properties of the soil, it was found that the sampling sites with pH < 8 (low calcium content) the preferential adsorption was a dominant process. This causes radium enrichment in organic matter and clay, which directly influence the soil gas radon activity concentration. At pH > 8, radium is no longer preferentially adsorbed on organic matter but continues to be adsorbed on clays albeit this process is weak because radium competes with calcium cations. Also, there are other factors that may affect radon emanation in soil such as radium concentration and distribution, porosity and water content. In contrast, empirical model of soil gas permeability overestimates the measured value in the study area by an order of magnitude. A new model was made by modifying the previously proposed one, which can be used as a guide for the estimation of the median value of soil gas permeability in granitic areas, but not as an accurate predictor due to the lack of correlation between the estimated and measured values.

Activity concentration of 137Cs in undisturbed attic dust collected from Salgótarján and Ózd (northern Hungary).

Due to the Chernobyl nuclear power plant accident, contaminated air masses, containing 137Cs, were widely propagated across all of Europe. Cesium-137 is easily adsorbed on aerosol particles as it returns to the lithosphere/pedosphere/via wet and dry deposition in the form of a radioactive fallout component. Following the nuclear accident, primary attention was paid to agricultural areas and less to urban environments. Our 137Cs activity study using undisturbed attic dust samples has been carried out from two residential areas (city of Salgótarján and Ózd) in northern Hungary, approx. 1000 km away from Chernobyl. A total of 61 attic dust samples were collected in 2016 and 2018 from houses (>30 years) functioning as family house, kindergarten, blockhouse and church. Activity concentration of 137Cs was determined for 1-2 g homogenized (<125 µm) attic dust samples in a low background iron chamber with a well-type HPGe detector. The mean 137Cs activity concentrations in attic dust samples are 88.5 ± 5.1 Bq kg-1 and 87.8 ± 4.5 Bq kg-1 in Salgótarján and Ózd, respectively. The dependence between 137Cs activities and the age of the houses was found to be significant (p=0.02), which could be explained by Chernobyl nuclear accident-causing elevated activity concentrations in location built prior to the accident. Three outliers in Ózd (>223 Bq kg-1), are probably related to the first rainfall event after the Chernobyl accident. Isotopic landscapes (isoscapes) of 137Cs were derived for both cities by means of kriging interpolation. In Salgótarján the 137Cs activity concentrations were higher than in Ózd which might have been due to redistribution loadings and local topographical features. We concluded that components of attic dust are highly useful indicators of home exposure to pollution events and remain detectable after several decades.

Spatial relationship between the field-measured ambient gamma dose equivalent rate and geological conditions in a granitic area, Velence Hills, Hungary: An application of digital spatial analysis methods.

In order to estimate the annual dose that the public receive from natural radioactivity, the identification of the potential risk areas is required which, in turn, necessitates understanding the relationship between the spatial distribution of natural radioactivity and the geogenic risk factors (e.g., rock types, presence of dikes, faults, physical conditions of soil, etc.). A detailed spatial analysis of outdoor ambient gamma dose equivalent rate was performed in the western side of Velence Hills, the largest outcropped granitic area in Hungary. In order to assess the role of local geology in the spatial distribution of gamma dose rates, field measurements were carried out at ground level at 300 sites along a 250 m x 250 m regular grid in a total surface of 19.8 km2. Digital image processing methods were applied to identify anomalies, heterogeneities and spatial patterns in the measured gamma dose rates, including local maxima and minima determination, digital cross sections, gradient magnitude and gradient direction, second derivative profile curvature, local variability, lineament density, 2D autocorrelation and directional variogram analyses. Statistical inference shows that different gamma dose rate levels are associated with the geological formations, with the highest level on the Carboniferous granite including outlying values. Moreover, digital image processing reveales that linear gamma dose rate spatial features are parallel to the SW-NE dike system and to the NW-SE main fractures. The results of this study underline the importance of understanding the role of geogenic risk factors influencing the ambient gamma dose equivalent rate received by public. The study also demonstrates the power of the image processing techniques for the identification of spatial pattern in field-measured geogenic radiation.

Spatial analysis of ambient gamma dose equivalent rate data by means of digital image processing techniques.

A detailed ambient gamma dose equivalent rate mapping based on field measurements at ground level and at 1 m height was carried out at 142 sites in 80 × 90 km area in Pest County, Hungary. Detailed digital image processing analysis was carried out to identify and characterise spatial features such as outlying points, anomalous zones and linear edges in a smoothed TIN interpolated surface. The applied method proceeds from the simple shaded relief model and digital cross-sections to the more complex gradient magnitude and gradient direction maps, 2nd derivative profile curvature map, relief map and lineament density map. Each map is analysed for statistical characteristics and histogram-based image segmentation is used to delineate areas homogeneous with respect to the parameter values in these maps. Assessment of spatial anisotropy is implemented by 2D autocorrelogram and directional variogram analyses. The identified spatial features are related to underlying geological and tectonic conditions using GIS technology. Results show that detailed digital image processing is efficient in revealing the pattern present in field-measured ambient gamma dose equivalent rates and they are related to regional scale tectonic zones and surface sedimentary lithological conditions in the study area.

Mapping geogenic radon potential by regression kriging.

Radon ((222)Rn) gas is produced in the radioactive decay chain of uranium ((238)U) which is an element that is naturally present in soils. Radon is transported mainly by diffusion and convection mechanisms through the soil depending mainly on the physical and meteorological parameters of the soil and can enter and accumulate in buildings. Health risks originating from indoor radon concentration can be attributed to natural factors and is characterized by geogenic radon potential (GRP). Identification of areas with high health risks require spatial modeling, that is, mapping of radon risk. In addition to geology and meteorology, physical soil properties play a significant role in the determination of GRP. In order to compile a reliable GRP map for a model area in Central-Hungary, spatial auxiliary information representing GRP forming environmental factors were taken into account to support the spatial inference of the locally measured GRP values. Since the number of measured sites was limited, efficient spatial prediction methodologies were searched for to construct a reliable map for a larger area. Regression kriging (RK) was applied for the interpolation using spatially exhaustive auxiliary data on soil, geology, topography, land use and climate. RK divides the spatial inference into two parts. Firstly, the deterministic component of the target variable is determined by a regression model. The residuals of the multiple linear regression analysis represent the spatially varying but dependent stochastic component, which are interpolated by kriging. The final map is the sum of the two component predictions. Overall accuracy of the map was tested by Leave-One-Out Cross-Validation. Furthermore the spatial reliability of the resultant map is also estimated by the calculation of the 90% prediction interval of the local prediction values. The applicability of the applied method as well as that of the map is discussed briefly.

Mapping the geogenic radon potential: methodology and spatial analysis for central Hungary.

A detailed geogenic radon potential (GRP) mapping based on field soil gas radon and soil gas permeability measurements was carried out in this study. A conventional continuous variable approach was used in this study for GRP determination and to test its applicability to the selected area of Hungary. Spatial pattern of soil gas radon concentration, soil permeability and GRP and the relationship between geological formations and these parameters were studied by performing detailed spatial analysis. Exploratory data analysis revealed that higher soil gas radon activity concentration and GRP characterizes the mountains and hills than the plains. The highest values were found in the proluvial-deluvial sediments, rock debris on the downhill slopes eroded from hills. Among the Quaternary sediments, which characterize the study area, the fluvial sediment has the highest values, which are also located in the hilly areas. The lowest values were found in the plain areas covered by drift sand, fluvioeolic sand, fluvial sand and loess. As a conclusion, radon is related to the sediment cycle in the study area. A geogenic radon risk map was created, which assists human health risk assessment and risk reduction since it indicates the potential of the source of indoor radon. The map shows that low and medium geogenic radon potential characterizes the study area in central Hungary. High risk occurs only locally. The results reveal that Quaternary sediments are inhomogeneous from a radon point of view, fluvial sediment has medium GRP, whereas the other rock formations such as drift sand, fluioeolic sand, fluvial sand and loess, found in the study area, have low GRP.

Dynamics of soil gas radon concentration in a highly permeable soil based on a long-term high temporal resolution observation series.

This paper studies the temporal variation of soil gas radon activity concentration in a highly permeable (k = 2.0E-11 m(2)) sandy-gravelly soil in order to understand if temporal variation of soil gas radon activity concentration can affect geogenic radon potential determination. Geogenic radon potential provides information about the potential risk from radon. Its calculation takes into account the equilibrium, saturated at infinite depth, soil gas radon activity concentration (c∞). This concentration may vary at annual time scale due to the environmental conditions. A long-term (yearly) and high temporal resolution (15 min) observation, applied in this study, reveal various temporal features such as long-term trend, seasonality, daily periodicity and sudden events in soil gas radon time series. Results show seasonal and daily periodical variation of the measured soil gas radon activity concentration (csoilRn) in a highly permeable sandy-gravelly soil with definite seasons without obvious long transitional periods. The winter (from October 2010 to April 2011) is characterized by 2.5 times higher average soil gas radon activity concentration (median is 7.0 kBq m(-3)) than the summer (August, September 2010 and May, June, July 2011) (median is 2.8 kBq m(-3)). Daily periodicity, which is much less than the seasonal one, controls the soil gas radon activity concentration mainly in the summer season. Average (AM) value of csoilRn is higher at night than in the daytime with about 18% and 3.8% in summer and in winter, respectively. As a conclusion, in case of single csoilRn measurement on a highly permeable (k ≥ 2.0E-11 m(2)) soil, similar to our test site, csoilRn should be corrected according to the seasons for calculating the equilibrium activity concentration c∞ value.

Cesium-137 concentration of soils in Pest County, Hungary.

This paper presents the results of measurements of (137)Cs in soils in Pest County, Hungary. We investigated forty five soil monoliths from monitoring locations of a countrywide Soil Information and Monitoring System (SIMS) at depths of 0-30, 30-60, 60-90, 90-120 and 120-150 cm. The (137)Cs concentrations were determined by gamma spectroscopy. We found that only the upper layer of soil (0-30 cm) contained (137)Cs above the detection limit (0.5 Bq kg(-1)). The (137)Cs concentration values ranged from the detection limit to 61.1 Bq kg(-1) ± 2.2 Bq kg(-1) and were lognormally distributed. The concentrations had a geometric mean 6.4 Bq kg(-1) and a geometric standard deviation 2.3 (an arithmetic mean 9.5 Bq kg(-1), an arithmetic standard deviation 11.3 Bq kg(-1)). We constructed a (137)Cs map for Pest County this is the first detailed (137)Cs map in Hungary. Concentrations were systematically higher (10.0-61.1 Bq kg(-1)) than average in the Pilis and Buda Mountains and the Northern part of the Gödöllo Hills. In contrast, low concentrations (0.0-10.0 Bq kg(-1)) characterized the southern part of the Gödöllo Hills, the Pest Plane and the Börzsöny Mountains. Two highest values were 46.9 Bq kg(-1) and 61.1 Bq kg(-1): one of these localities, a loamy brown forest soil was chosen to study relationship between (137)Cs migration and clay materials of the soil. According to differential thermal analysis (DTA) and x-ray diffraction (XRD) analyses, illite and kaolinite were dominant in the soil. The amount of clay was closely proportional to (137)Cs concentration (R = 0.89). At the locality having the highest surface concentration, 78% of the total detected (137)Cs concentration was measured in the top 3 cm layer of soil profile and there was no detectable concentration below 20 cm. This result indicates that penetration of (137)Cs into the soil is a very slow process in this case. Analysis of this depth profile showed lower (137)Cs migration parameter values (effective diffusion coefficient and migration velocity) than predicted in a previous study for brown forest soils in the same area of Hungary.