AC Andrello

AZ Hrynkiewicz

B Kubica

B. Kubica

BS Samat

C Papastefanou

H Bem

K. Szarlowicz

LI Tsikritzis

M. Stobinski

MA Shenber

R Misiak

S Skiba

W. Reczynski

Crossref

The evaluation of 137Cs radioactivities in soils takenfrom the Babia Go´ra National ParkM. Stobinski • K. Szarlowicz • W. Reczynski •B. KubicaReceived: 22 July 2013 / Published online: 5 November 2013 The Author(s) 2013. This article is published with open access at Springerlink.comAbstract The aim of this work was to determine 137Cs and40K radioactivities in soil samples taken from the Babia Go´raNational Park (BPN) in south Poland. The cluster analysis(CA) and principal component analysis (PCA) were used todiscuss the obtained data. 10 cm thick soil cores were col-lected from the BPN area. Each sample was divided intothree sub-samples. The samples were dried, homogenizedand packed in polyethylene containers. The radioactivities of137Cs and 40K were measured by means of gamma spec-trometry. It was found that 137Cs radioactivity in the whole10 cm soil cores was in the range from 1,916 to28,551 Bq m-2. The radioactivity of 40K varied from 1,642to 25,654 Bq m-2. Using CA it was possible to diverse thesoils taking into account soil types. By use of the PCAmethod, it was chosen three factors which are appropriate tocharacterize researched parameters.Keywords 137Cs  Babia Go´ra National Park  Soilcores  Cluster analysis  Principal componentanalysisIntroductionMountainous ecosystems are highly sensitive to any distur-bances in natural balance, what makes them especiallyinteresting for observations of chemical and radiochemicalcontamination. The area of the Babia Go´ra National Park(BPN), being located along the main ridge of the FlyschCarpathian Mountains, is just the proper place in this respect.The terrain belongs to the young folded mountains, builtmainly of flysch and some other lithology. The area is char-acterized by highly variable and unique natural resources.The highest summit of the Babia Go´ra Mountain’s massif(west part of the Beskid _Zywiecki chain of mountains) isDiablak reaching 1,725 m asl. To protect this unique area theBPN and the UNESCO World’s Biosphere Reserve wereestablished. The area of the BPN, like other regions of Poland,was exposed to substantial contamination with radionuclidesdue to the Chernobyl accident in 1986 and nuclear weapontests since the fifties of the twentieth century [1–6]. Resear-ches on radionuclides distribution in the environment areimportant not only because these are perfect markers of theenvironment pollution but also because radioactive isotopesare not immobilized in soil but are constantly interchangedbetween inorganic matter and living organisms [7].The aim of the work was to establish the spatial distri-bution of c-radionuclides i.e. anthropogenic 137Cs (T1/2 =30.07 years) and natural 40K (T1/2 & 109 years) in the soilsamples collected in the described above area.Materials and methods10 cm thick soil core samples were collected with the useof a cylindrical corer (10 cm in diameter). 13 samplingPaper presented during the 6th All Polish Conference onRadiochemistry and Nuclear Chemistry, Krakow (Poland), 21–24April 2013.M. Stobinski (&)  K. Szarlowicz  B. KubicaFaculty of Energy and Fuels, AGH University of Science andTechnology, al. A. Mickiewicza 30, 30-059 Krako´w, Polande-mail: marcin.stobinski@agh.edu.pl; stobinsk@agh.edu.plW. ReczynskiFaculty of Material Science and Ceramics, AGH University ofScience and Technology, A. Mickiewicza 30, 30-059 Krako´w,Poland123J Radioanal Nucl Chem (2014) 299:631–635DOI 10.1007/s10967-013-2809-zpoints were selected in the studied area, most of themlocalized along the mountains’ main ridge. Each of thesampling points was described by its geographical coor-dinates and height above the sea level. In case of few pointsit was impossible to determine their precise coordinates(the lack of GPS signal), so the closest available coordi-nates were interpolated. In the laboratory, the cores weredivided into three sub-samples each to enable radioisotopesdetermination in various depths. The core sub-sampleswere marked as follows—‘‘a’’ (0–3 cm), ‘‘b’’ (4–6 cm) and‘‘c’’ (7–10 cm). The samples were then dried at 105 C andthe total weight was determined. After removal of organicmacro-particles and small stones, the samples were sievedmechanically (2 mm mesh).After preparation, the samples were analysed by meansof gamma ray spectrometry with the use of HPGe (highpurity germanium) coaxial detectors of relative efficiency 7and 21 %. Prior to the measurements, the soil density wasdetermined for further use in calibration corrections cal-culations [8]. Each measurement lasted 72 h. The referencematerials IAEA-154, IAEA-375, and IAEA-447 of theInternational Atomic Energy Agency (Vienna, Austria)were used in the measurements. In the present work 137Csradioactivity in the ‘‘a’’ soil layer was given in Bq kg-1units. For the whole core samples, 137Cs and 40K activitieswere expressed in Bq m-2 units. All given caesiumradioactivity values were recalculated for the day01.09.2010. After gamma spectrometric measurementsorganic matter content in the soil samples was determinedby means of incineration at 600 C.To extract relevant information out of the obtained data,the data matrix consisting of all analysed features of allsamples was analysed statistically. Chemometric tools i.e.cluster analysis (CA) and principal components analysiswere used (using Statistica 10 software).Results and discussionThe sampling points description is given in Table 1. Theresults of radioisotopes activity and soil density are presentedin Table 2. The most important values are written in bold.Soil in the BPN originates from the Carpathian Flyschwaste. As in the area vegetation levels are well distinguished,for each sampling point the soil type can be attributed. Theresulting soil type classification is given in Table 3 [9].Chemometric tools are widely used in the environmentaldata analysis especially when high variability and uncer-tainty of the data may be expected [10]. For the obtainedset of data the CA according to Ward and principal com-ponents analysis (PCA) after initial normalization/auto-scaling, were used. The outcome of the analyse is presentedin Figs. 1 and 2.In Fig. 1 the dendrogram of the variables similarity isanalysed. Two main clusters are distinguished—the firstone represents soil density and 40K radionuclide activity(40K activity is in constant relation to the total potassium,about 31 Bq 40K per 1 g of potassium [11]).These two variables belong to the same cluster whatsuggests that potassium is incorporated mainly in mineralcomponents of the soil. The higher is mineral content ofsoil, the higher is soil density (Table 2). In the secondcluster, radioactivities of artificial 137Cs in the ‘‘a’’ soillayer and in the whole core as well as the sampling pointheight asl and organic matter content, are grouped.Similar course of changes of 137Cs activity and soilorganic matter content can be attributed to the sorptiveproperties of this soil fraction. As 137Cs presence in the soilresults only from the distant transport of the contaminant, itsretention in soil is a direct result of its sorption. The otherimportant factor is the amount of precipitation in the area(rain, snow). The higher is the location of the sampling pointin the mountains, the higher is the amount of precipitation.Thus, the variable—altitude—belongs to the same cluster.Table 1 The Babia Go´ra National Park sampling points descriptionPointno.GeographicalcoordinatesHeight(m asl)Place description1 N 49st 34,797 1,515 Red hiking trail, after Sokolica,right from this red routeE 19st 33,4142 N 49st 34,616 1,577 Near Zimny Staw Lake,at the top of Babia Go´raE 19st 32,7723 N 49st 34,341 1,707 By green hiking trail from BabiaGo´ra to LipnicaE 19st 31,8244 N 49st 34,426 1,701 The yellow hiking trail fromBabia Go´ra, on the right sightof this routeE 19st 31,7695 N 49st 34,386 1,695 The route from Diablak (redhiking trail)E 19st 31,6896 No data 1,600 The route from Diablak belowCross (red hiking trail)7 No data 1,530 Krzy _zo´wka szlako´w na MarkoweSzczawiny i Mała˛ Babia˛.8 No data 950 Mokry Stawek Lake, from thesite of Krowiarki Pass9 No data 951 Brona Pass10 N 49st 34,528 1,463 By yellow hiking trail, dwarfpine zoneE 19st 31,45311 N 49st 34,667 1,350 Yellow hiking trail, at the end ofhigher montane zoneE 19st 31,30112 N 49st 34,953 1,257 At the intersection of Szumia˛cawoda Valley with the route toMarkowe SzczawinyE 19st 31,46713 N 49st 34,293 836 Hala S´mietanowa, above littlebridge on Syhlec streamE 19st 35,609632 J Radioanal Nucl Chem (2014) 299:631–635123In Fig. 2 the similarity of sampling points is presented.The clusters group points not necessarily close to eachother. But the chosen criteria i.e. analysed variables,enabled proper and logical division of the sampling pointsinto groups (clusters) for which the soil type is a commonfeature (Table 3). However, it should be noted that inmountains, soil types are not sharply defined. As a resultthe revealed clusters do not classify soil types directly, butthe obtained classification is relevant for a given soilcomplex structure (Fig. 2; Table 3).In further statistical analysis of the obtained results, theprincipal components analysis was performed. Principalcomponents are the linear combination of the previousvariables.Taking into consideration the Kaiser criterion in furtheranalysis only the first and the second principal componentshould be used (Table 4). The scree diagram suggestsTable 2 137Cs and 40K radioactivities, density and organic matter content in the soil samples collected in the Babia Go´ra National Park areaPoint no. Height(m asl)Soil density(g cm-3)Organic mattercontent (%)Activity 137Cs(Bq kg-1) (layer ‘‘a’’)Activity 137Cs(Bq m-2) (whole core)Activity 40K(Bq m-2) (whole core)1 1,515 0.70 17 416 ± 11 8,837 ± 241 6,900 ± 6192 1,577 0.17 90 405 ± 16 3,757 ± 211 4,127 ± 3743 1,707 0.55 20 304.1 ± 9.2 6,591 ± 224 7,914 ± 7154 1,701 0.65 15 831 ± 21 28,551 ± 720 16,477 ± 1,4975 1,695 0.70 14 246.2 ± 8.4 8,166 ± 275 10,848 ± 9776 1,600 0.24 73 697 ± 21 7,231 ± 219 2,134 ± 1947 1,530 0.22 81 214 ± 10 3,276 ± 177 7,869 ± 7138 950 0.99 9 36.8 ± 2.1 1,783 ± 119 25,654 ± 2,2889 951 0.,70 37 65.8 ± 6.4 2,119 ± 152 12,907 ± 1,16410 1,463 0.50 21 137.3 ± 6.1 1,916 ± 83 8,368 ± 77511 1,350 0.57 19 309 ± 10 5,472 ± 230 25,200 ± 2,25512 1,257 0.17 82 326 ± 15 2,030 ± 95 1,642 ± 15113 836 0.40 23 408 ± 13 16,152 ± 484 17,480 ± 1,573Table 3 Prevailing soil types of the considered sampling pointsVegetationlevelHeight(m asl)Prevailing soil type SamplingpointsAlpine zone 1,650–1,725 Lithic Leptosol, 3, 4, 5Regosol Skeletic,Podzolic Ranker(Leptosol)Dwarf pinezone1,390–1,650 Haplic Podzol, 1, 2, 6, 7,10Tangel–Ranker(Umbric Leptosol)Highermontane zone1,150–1,390 Dystric Cambisol 12, 11Partially HaplicPodzolLower montanezone700–1,150 Eutric and DystrictCambisol13, 8, 9Ward's methodActivity 40K [Bq/m2]Density [g/cm3]Organic matter [%]Activity 137Cs [Bq/m2]Activity 137Cs [Bq/kg]Altitude [m.asl]123456789Euclidean distanceFig. 1 Cluster analysis (variables). Activity of 137Cs [Bqm-2]represents activity in the whole profile; activity of 137Cs [Bqkg]represents activity in ‘‘a’’ layerWard's method6 12 7 2 13 11 9 8 4 10 5 3 1Sampling point024681012Euclidean distanceFig. 2 Cluster analysis (samples)J Radioanal Nucl Chem (2014) 299:631–635 633123however, that it would be reasonable to consider threecomponents as they describe 92.36 % of global variation ofthe data (Fig. 3).In Table 5 factor loadings (after varimax rotation) forthe three principal components are given.The first component (explaining 46 % of variability)covers mainly the following variables: density, organicmatter content and potassium concentration. All theseparameters are connected with the physical properties andchemical composition of the soil. The second principalcomponent, explaining 33 % of variability, considers onlyanthropogenic variable i.e. radioactivity of 137Cs. Thirdprincipal component explaining 13 % of variability refersto the height asl of the sampling point. It should be stres-sed, that this component supplies additional informationrelated to some aspects explained by the first two principalcomponents. The height above sea level has the influenceon such soil properties like density and organic mattercontent. With increasing altitude the pace of organic matterdecomposition decreases (the same tendency is noted fortemperature). Simultaneously, anthropogenic 137Cs wasintroduced to the soil mainly with rainfall—in the moun-tains, the higher located is the place the more rain isprecipitated.In Fig. 4 it may be noted that the variables (soil densityand potassium content) are positively correlated witch eachother and negatively correlated with organic matter con-tent. On the other hand it is clear that 137Cs radioactivity isorthogonal to those variables (soil density and potassiumcontent)—no correlation was found.ConclusionsIt was established that:• Caesium radioactivity in the soils of the BPN ischangeable. In the top (‘‘a’’ layer) 3 cm thick soil layerit is in the range from 36 to 831 Bq kg-1, while in thewhole core (10 cm) it spans from 1,916 to28,551 Bq m-2. CA enabled grouping of the samplingpoints according to the soil type. It may be assumedScree diagramEigenvalues46,4739%32,7826%13,1060%4,2274%2,1176%1 2 3 4 5Number  of  eigenvalues-0,50,00,51,01,52,02,53,03,5ValueFig. 3 Scree diagramTable 4 EigenvaluesPrincipal components analysisEigenvalues % totalvarianceCumul.-eigenvalueCumul.-%1 2.79 46.48 2.79 46.482 1.97 32.78 4.76 79.263 0.79 13.10 5.55 92.364 0.25 4.23 5.80 96.595 0.13 2.12 5.93 98.716 0.07 1.29 6.00 100.00Table 5 Factor loadings (varimax)VF-1 VF-2 VF-3Altitude -0.090 0.232 0.942Density 0.950 -0.107 -0.096Radioactivity of 137Cs (‘‘a’’ layer) -0.235 0.906 0.271Radioactivity 40K 0.721 0.094 -0.556Radioactivity 137Cs (whole core) 0.247 0.945 0.025Organic matter 20.956 -0.108 0.050Significant values are given in boldAltitude [m.asl]DensityActivity 137Cs [Bq/kg]Activity 40K [Bq/m2]Activity 137Cs [Bq/m2]Organic matter [%-1,0 -0,5 0,0 0,5 1,0Factor 1 : 46,5%-1,0-0,50,00,51,0Factor 2 : 33%]Fig. 4 Projection of the variables onto the plane of the first twoprincipal components634 J Radioanal Nucl Chem (2014) 299:631–635123that the sampling points are better characterized by the137Cs radioactivity expressed in surface units ratherthan radioactivity of the first layer only.• The PCA reduced the number of analysed variables tothree principal components, explaining 92 % of thetotal variance of the variables. First three principalcomponents differentiate the variables into: natural(connected with physical and chemical soil properties)like soil density, organic matter and potassium con-tents, anthropogenic—137Cs radioactivity, and sam-pling points characteristic—altitude above sea level.Presented above conclusions are concomitant with theresults of research performed in the similar mountainousecosystems. It is true especially for the neighbouring TatraMountains National Park [3, 5, 12]. The similar positivecorrelation of 137Cs activity with the sampling point alti-tude and organic matter content in the soil were found inthe Tatras. Similarly the soil density was correlated withpotassium content.Soils of the mountains neighbouring to the BPN constitutecurrently the subject of complementary research projects.Acknowledgments The work was supported by the NCN Grant No.N N304 17040 and the AGH University of Science and TechnologyGrant No. 11.11.210.244.Open Access This article is distributed under the terms of theCreative Commons Attribution License which permits any use, dis-tribution, and reproduction in any medium, provided the originalauthor(s) and the source are credited.References1. Bem H (2005) Radioactivity in the natural environment. PAN,Ło´dz´ (in Polish)2. Hrynkiewicz AZ (2001) Man and the ionization radiation. WNPWN, Warszawa (in Polish)3. Kubica B, Mietelski JW, Gołas´ J, Skiba S, Tomankiewicz E,Gaca P, Jasin´ska M, Tuteja-Krysa M (2002) Concentration of137Cs, 40K, 238Pu and 239?240Pu radionuclides and some heavymetals in soil samples from two main valleys from the TatraNational Park. 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Zeszyty Naukowe UJ Prace Geograficzne98:189–19810. Tsikritzis LI (2005) Chemometrics of the distribution and originof 226Ra, 228Ra, 40K and 137Cs in plants near the West MacedoniaLignite Center (Greece). J Radioanal Nucl Chem 264:651–65611. Samat BS, Green S, Beddoe AH (1997) The 40K activity of onegram of potassium. Phys Med Biol 42:407–41312. Kubica B, Skiba S, Drewnik M, Stobin´ski M, Kubica M, Gołas´M, Misiak R (2010) Radionuklides 137Cs and 40K in the soils ofthe Tatra National Park (TPN, Poland). Nukleonika 55:377–386J Radioanal Nucl Chem (2014) 299:631–635 635123

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The evaluation of 137Cs radioactivities in soils taken from the Babia Góra National Park

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The evaluation of 137Cs radioactivities in soils taken from the Babia Góra National Park

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