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222Rn Concentration in Groundwaters Circulating in Granitoid Massifs of Poland

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222Rn Concentration in Groundwaters Circulating in Granitoid Massifs of Poland water Article 222Rn Concentration in Groundwaters Circulating in Granitoid Massifs of Poland Tadeusz A. PRZYLIBSKI 1,* , El˙zbietaDOMIN 1, Joanna GORECKA 2 and Agata KOWALSKA 1 1 Faculty of Geoengineering, Mining and Geology, Wrocław University of Science and Technology, Wybrze˙zeS. Wyspia´nskiego27, 50-370 Wrocław, Poland; [email protected] (E.D.); [email protected] (A.K.) 2 ul. Konopnickiej 17, 51-141 Wrocław, Poland; [email protected] * Correspondence: [email protected] Received: 21 January 2020; Accepted: 6 March 2020; Published: 9 March 2020 Abstract: The authors’ research has shown that the maximum values of 222Rn activity concentration in all granitoid massifs of Poland exceed 100 Bq L 1, i.e., the value allowed for waters intended · − for human consumption. Such waters should be de-radoned prior to being distributed through the water supply networks. Even more common in these areas is the occurrence of potentially medicinal radon waters, i.e., waters characterized, in accordance with Polish law, by radon activity concentration of at least 74 Bq L 1. Such waters may be used for balneotherapeutic treatments. · − For the Karkonosze, Strzegom-Sobótka, Kłodzko-Złoty Stok and Kudowa massifs, the range of hydrogeochemical background of 222Rn exceeds both 74 and 100 Bq L 1. This indicates common · − occurrence in these areas of both potentially medicinal radon waters and waters which require de-radoning before being supplied for human consumption. More than 50% of groundwaters from the Karkonosze granite area contain over 100 Bq L 1 of 222Rn. This means that these waters are · − mostly radon and high-radon waters. The remaining massifs contain predominantly low-radon waters and radon-poor waters. The 222Rn concentrations obtained by the authors are comparable to values measured in groundwaters in other granitoid massifs in the world, creating both problems and new application possibilities. Keywords: radon; groundwater; radon water; tap water; medicinal water; granite; granitoid; hydrogeochemical background 1. Introduction The radon isotope 222Rn, alongside radium isotopes 226Ra and 228Ra, is the most important natural component of groundwaters, giving them their radioactive properties [1,2]. 222Rn is a natural radioactive isotope whose activity concentration in groundwaters varies in a very broad range—from 10 4 Bq L 1 to 102,000 Bq L 1, hence reaching 9 orders of magnitude [3]. Among the four natural − · − · − isotopes of radon (with mass numbers 222, 220, 219 and 218), it is only 222Rn that, owing to its half-life of slightly more than 3.82 days [4–6], can be transported with groundwater over distances of dozens or even hundreds of metres, and occasionally even further [2,7]. This is the reason for common occurrence of 222Rn in groundwater environment [3,8,9]. The activity concentration of this gas in groundwater is mainly due to the parent 226Ra content in the reservoir rock and the emanation coefficient of this rock [2,10,11] enabling the 222Rn formed in it to be released from the structures of rock minerals and grains containing 226Ra, and then dissolved in water. Therefore, the highest concentrations of radon could be expected in groundwaters flowing through granitoid reservoir rocks. Radon-enriched waters occur particularly in areas of strong brittle tectonic deformations and in zones of fractures and Water 2020, 12, 748; doi:10.3390/w12030748 www.mdpi.com/journal/water Water 2020, 12, 748 2 of 16 weathering alterations, hence at small depths of the order of several dozen meters under the ground surface [2,11,12]. From the point of view of radiological protection, 222Rn present in groundwater in concentrations higher than 100 Bq L 1 is hazardous to human health and it should be removed from water before it is · − used for human consumption. This issue is regulated by appropriate European Union legislation [13], which was the basis for setting this parametric value also in Polish law [14]. At the same time, numerous radon health resorts around the world offer balneotherapeutic treatments using radon waters [12,15–21]. In Poland, groundwaters with 222Rn activity concentration of at least 74 Bq L 1 can · − be regarded as medicinal in light of geological and mining law [22]. In areas built of granitoid rocks, one can expect the occurrence of radon-enriched waters. This calls for thorough assessment of radon concentration in groundwaters occurring in these areas. On the one hand, it is essential to prevent residents’ exposure to increased effective doses of ionizing radiation from radon released from water and inhaled together with its radioactive decay products, isotopes of 218,214,210Po, 214,210Bi, 214,210Pb and 210,206Tl, formed in the air. On the other hand, this information may be significant for medicinal and balneotherapeutic procedures based on the extraction and exploitation of radon-enriched waters in health resorts [12]. The aim of the authors’ research is the assessment of the range of 222Rn content in groundwaters occurring in these areas of Poland whose geological structure is dominated by granitoid rocks. This information is essential for the needs of groundwater usage planning in these areas and effective radiological protection of their inhabitants. 2. Research Area In Poland, areas with geological structures dominated by granitoid massifs are found in the south-western and the southern parts of the country (Figure1). So far, it is mainly the area of Lower Silesia, i.e., the south-western part of the country, where research into radon occurrence in the natural environment has been conducted [23]. The geological structure of this part of Poland is the reason for the occurrence of locally high or very high concentrations of radon. The south-western part of Poland is made up of the so-called Lower Silesian block, whose southern part is composed of the Sudety mountain ranges, and the northern part—of foothills forming the geological structures of the so-called Fore-Sudetic block. These two parts are separated from each other by a regional tectonic dislocation–the Sudetic marginal fault. This region constitutes the north-eastern part of the crystalline Bohemian massif, one of major massifs built of crystalline (igneous and metamorphic) rocks in Europe [24–26]. The structure of this area is characterized by the occurrence at small depths or on the surface of uranium-enriched crystalline rocks, including granitoid massifs [2,23,27,28]. In about a dozen places in the area of the Sudetes, usually small and now unexploited uranium deposits have been documented [29–32]. This is the reason why Lower Silesia is the only area in Poland for which a map of radon potential has been created [33]. The groundwaters of this area have been the main subject of numerous research works on hydrogeochemistry of 222Rn and its parent 226Ra [34–46]. Also, detailed research has been conducted into the occurrence of 222Rn in groundwaters flowing through granitoid rocks of three Variscan massifs located in the Sudetes [47]. Water 2020, 12, 748 3 of 16 Water 2020, 12, x FOR PEER REVIEW 3 of 16 FigureFigure 1. 1.Location Location of of granitoid granitoid massifs massifs on on a a simplified simplified tectonic tectonic map map of of Poland Poland without without Cainozoic Cainozoic depositsdeposits (according (according to [48to –[48–50];50]; slightly slightly modified). modified 1–Karkonosze). 1 – Karkonosze granite, 2–Strzegom-Sobgranite, 2 – Strzegom-Sobótkaótka granitoid, 3–Kudowagranitoid, granitoid,3 – Kudowa 4–Kłodzko-Złoty granitoid, 4 – StokKłodzko-Z granitoid,łoty 5–StrzelinStok granitoid, granitoid, 5 – Strzelin 6–Tatra granitoid, granitoid. 6 – Tatra granitoid. The authors are currently continuing research into 222Rn occurrence in groundwater environment. The analysisThe authors of results are obtainedcurrently so farcontinuing has resulted research in a decisioninto 222Rn to extendoccurrence the researchin groundwater onto all granitoidenvironment. massifs The in Poland.analysis Theof result authors’s obtained research so is far mainly has resulted focused in on a fivedecision areas to of extend Variscan the granitoid research occurrenceonto all granitoid in Lower massifs Silesia, in which Poland. has The considerably authors’ rese broadenedarch is mainly the current focused knowledge on five areas of this of problem Variscan presentedgranitoid byoccurrence Przylibski in and Lower Gorecka Silesia, [47 which]. Moreover, has considerably this is the firstbroadened time that the researchcurrent knowledge has covered of thethis area problem of Variscan presented granitoids by Przylibski of the Tatras,and Gorecka building [47] the. Moreover, inner part this of is the the Carpathians, first time that an research alpine orogenhas covered [51,52]. the area of Variscan granitoids of the Tatras, building the inner part of the Carpathians, an alpine orogen [51,52]. 3. Methods of Measurements and Result Calculation 3. MethodsOver the of course Measurements of fieldwork, and the Result authors Calculation collected groundwater samples from accessible springs and wells (usually shallow dug wells), and occasionally also from accessible deep drilled wells. Over the course of fieldwork, the authors collected groundwater samples from accessible springs In mountain areas, i.e., in the areas of the Karkonosze granite massif and of the Tatra granitoids, water and wells (usually shallow dug wells), and occasionally also from accessible deep drilled wells. In samples were taken chiefly from springs. In the area of Kudowa granitoids, the proportions of springs mountain areas, i.e. in the areas of the Karkonosze granite massif and of the Tatra granitoids, water and wells in water sampling were comparable while in the remaining granitoid massifs (Kłodzko-Złoty samples were taken chiefly from springs. In the area of Kudowa granitoids, the proportions of springs Stok, Strzelin and Strzegom-Sobótka), most groundwater samples were taken from wells. and wells in water sampling were comparable while in the remaining granitoid massifs (Kłodzko- Złoty Stok, Strzelin and Strzegom-Sobótka), most groundwater samples were taken from wells.
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