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The first national human biomonitoring in Slovenia surveyed cadmium (Cd), lead (Pb), mercury (Hg), arsenic (As), manganese (Mn), selenium (Se), copper (Cu) and zinc (Zn) in a childbearing population (18–49 years) selected from lactating primiparous women and men (N = 1084). The overall aim was to estimate trace elements' levels and geographical variations in order to identify sources of possible exposures and set the national reference values. The study population was selected evenly from 12 study areas across Slovenia, including rural, urban and known or potentially contaminated environments. Within 6–8 weeks after delivery, venous blood, spot urine, scalp hair and breast milk samples were collected to determine the selected elements. The data analysis included descriptive statistics and multiple linear regression using elemental concentrations in biological matrices, questionnaire data and environmental datasets. Essential elements showed no significant deficiencies or excessive levels in the study population and were largely determined by sex and/or the participating women's physiological status (postpartum, lactation), as well as by certain dietary sources. Toxic elements' levels were mainly below the levels considered to present increased health risk. Lifestyle and nutritional habits appeared as significant determinants of exposure to Cd (smoking and game meat consumption), Hg (seafood and amalgam fillings), As (seafood) and Pb (alcohol consumption, smoking, game meat consumption and type of water supply). A distinctive geographical pattern was confirmed, due to past mining activities combined with naturally elevated background levels in the cases of Pb (Mežica Valley), Hg (Idrija and Posocje) and As exposure (Zasavje). Increased seafood consumption in the coastal study area contributed to higher Hg and As (arsenobetaine) levels. Extensive sample size database accompanied with life-style and environmental data improved the prediction of exposure patterns, set the reference values for the childbearing population living in Slovenia, and provided a strong basis for evaluating spatial and temporal trends in exposure. To our best knowledge, this is the first study to establish reference values for lactating primiparous women.

The total activity of 210 Po was determined by alpha-spectrometry in various samples (matrices) collected in the Gulf of Trieste (northern Adriatic Sea) where fresh water inflows, especially from the Isonzo River in the northern part, affect water quality. Observed 210 Po levels were: 1) 0.56–3.75 mBq/L in the dissolved phase ( S transect in the gulf and sectioned to the depth of 20 cm) and 4) 239 (autumn) – 415 to 1800 (spring) Bq/kg (dw) in meso(zoo)plankton (>200 μm). In seawater and tributaries, up to 80% (mean 49%) of total 210 Po was found in particulate form. In sediments, slightly higher levels were encountered in the Isonzo prodelta and in the central (depocenter) part of the gulf. K D (L/kg) calculated between seawater and SPM, and seawater and sediment amounted to about 5 × 10 6 and 6 × 10 4 , respectively. Lower autumn 210 Po levels can be a consequence of biological dilution by higher mesozooplankton biomass in the autumn compared to spring. Plankton fractionation revealed in general the highest levels in the >200 μm mesoplankton fraction (239–1800 Bq/kg) followed by 50–200 μm (388–996 Bq/kg) and 20–50 μm (318–810 Bq/kg) microplankton fractions. Obtained data show higher 210 Po levels in all matrices analyzed in the Gulf of Trieste compared to other Adriatic (central Adriatic) and western Mediterranean areas. The 210 Po/ 210 Pb ratios in water, plankton and sediments were mostly below or around 1, while this ratio was much higher at higher trophic levels (up to about 50), reflecting a preferential bioaccumulation of 210 Po over 210 Pb. 210 Po accumulation between seawater and SPM and seawater and mesozooplankton amounted to 3.7 × 10 4 and 1.1 × 10 4 , respectively, similar to other Adriatic areas. Comparison of the relative importance of pelagic and benthic bioaccumulation pathways, excluding the filter feeder bivalves, suggests greater accumulation in pelagic-feeding species.

We monitored trace metals and nitrogen using naturally growing moss Hypnum cupressiforme Hedw. in urban and peri-urban forests of the City Municipality of Ljubljana. The aim of this study was to explore the differences in atmospheric deposition of trace metals and nitrogen between urban and peri-urban forests. Samples were collected at a total of 44 sites in urban forests (forests within the motorway ring road) and peri-urban forests (forests outside the motorway ring road). Mosses collected in urban forests showed increased trace metal concentrations compared to samples collected from peri-urban forests. Higher values were significant for As, Cr, Cu, Hg, Mo, Ni, Pb, Sb, Tl and V. Within the motorway ring road, the notable differences in element concentrations between the two urban forests were significant for Cr, Ni and Mo. Factor analysis showed three groups of elements, highlighting the contribution of traffic emissions, individual heating appliances and the resuspension of contaminated soils and dust as the main sources of trace elements in urban forests.

An assessment of the radiological situation due to exposure to radon and gamma emitting radionuclides was conducted in southern Kosovo. This study deals with sources of radon in soil gas. A long-term study of radon concentrations in the soil gas was carried out using the SSNTDs (CR-39) at 21 different locations in the Sharr-Korabi zone. The detectors were exposed for an extended period of time, including at least three seasonal periods in a year and the sampling locations were chosen with respect to lithology. In order to determine the concentration of the natural radioactive elements 238U and 226Ra, as a precursor of 222Rn, soil samples were collected from each measuring point from a depth of 0.8 m, and measured by gamma spectrometry. The levels (Bq kg-1) of naturally occurring radionuclides and levels (kBq m-3) of radon in soil gas obtained at a depth 0.8 m of soil were: 21-53 for 226Ra, 22-160 for 238U and 0.295-32 for 222Rn. With respect to lithology, the highest value for 238U and 226Ra were found in limestone and the highest value for 222Rn was found in metamorphic rocks. In addition, the results showed seasonal variations of the measured soil gas radon concentrations with maximum concentration in the spring months.

Tobacco and tobacco smoke are very complex mixtures. In addition to various chemical and organic compounds they also contain natural radioactive elements (radionuclides). In this work, the natural radionuclide activity concentrations ((234)U, (238)U, (228)Th, (230)Th, (232)Th, (226)Ra, (210)Pb and (210)Po) of nine different cigarette samples available on the Slovenian market are reported. In addition to (210)Po, the transfer of thorium isotopes from a cigarette to a smoker's body and lungs have been determined for the first time. Cigarette smoke and exhaled air from smokers' lungs were collected from volunteer smokers (C-4 brand) to determinate what quantity of (210)Po and thorium isotopes is transferred from the tobacco to the smoker's lungs. Cigarette ash and smoked filters were also collected and analysed. Among the determined isotopes, (210)Pb and (210)Po showed the highest activity concentrations. During the smoking of one cigarette approximately 22% of (210)Po (and presumably its predecessor (210)Pb), 0.6% of (228)Th, 24% of (230)Th, and 31% of (232)Th are transferred from the cigarette and retained in the smoker's body. The estimated annual effective dose for smokers is 61 μSv/year from (210)Po; 9 μSv/year from (210)Pb; 6 μSv/year from (228)Th; 47 μSv/year from (230)Th, and 37 μSv/year from (232)Th. These results show the importance of thorium isotopes in contributing to the annual effective dose for smoking.

Mosses were collected from 103 locations and analyzed for N concentration and δ 15 N values. At each location, the samples were collected from two types of site: under the tree canopies and in the adjacent forest openings. A spatial correlation was detected, and ordinary kriging could be applied only to the N in the mosses that were collected in the openings. In contrast, a spatial correlation was not detected for N in the mosses that were collected under the canopies or for the δ 15 N of the mosses at either type of site. For those, the spatial interpolation was calculated as the sum of the regression predictions and the inverse distance weighted interpolation of residuals. The maps for the N at both site types (canopy/open) identified similar areas with increased N concentrations. The sole exception was the mosses collected under the canopy, for which some local emitters of NO x were also identified.

Background This paper aims to investigate the correlations between the concentrations of nine heavy metals in moss and atmospheric deposition within ecological land classes covering Europe. Additionally, it is examined to what extent the statistical relations are affected by the land use around the moss sampling sites. Based on moss data collected in 2010/2011 throughout Europe and data on total atmospheric deposition modelled by two chemical transport models (EMEP MSC-E, LOTOS-EUROS), correlation coefficients between concentrations of heavy metals in moss and in modelled atmospheric deposition were specified for spatial subsamples defined by ecological land classes of Europe (ELCE) as a spatial reference system. Linear discriminant analysis (LDA) and logistic regression (LR) were then used to separate moss sampling sites regarding their contribution to the strength of correlation considering the areal percentage of urban, agricultural and forestry land use around the sampling location. After verification LDA models by LR, LDA models were used to transform spatial information on the land use to maps of potential correlation levels, applicable for future network planning in the European Moss Survey. Results Correlations between concentrations of heavy metals in moss and in modelled atmospheric deposition were found to be specific for elements and ELCE units. Land use around the sampling sites mainly influences the correlation level. Small radiuses around the sampling sites examined (5 km) are more relevant for Cd, Cu, Ni, and Zn, while the areal percentage of urban and agricultural land use within large radiuses (75–100 km) is more relevant for As, Cr, Hg, Pb, and V. Most valid LDA models pattern with error rates of

In recent decades, naturally growing mosses have been used successfully as biomonitors of atmospheric deposition of heavy metals and nitrogen. Since 1990, the European moss survey has been repeated at five-yearly intervals. In 2010, the lowest concentrations of metals and nitrogen in mosses were generally found in northern Europe, whereas the highest concentrations were observed in (south-)eastern Europe for metals and the central belt for nitrogen. Averaged across Europe, since 1990, the median concentration in mosses has declined the most for lead (77%), followed by vanadium (55%), cadmium (51%), chromium (43%), zinc (34%), nickel (33%), iron (27%), arsenic (21%, since 1995), mercury (14%, since 1995) and copper (11%). Between 2005 and 2010, the decline ranged from 6% for copper to 36% for lead ; for nitrogen the decline was 5%. Despite the Europe-wide decline, no changes or increases have been observed between 2005 and 2010 in some (regions of) countries.

International audience; AbstractKey messageMoss surveys provide spatially dense data on environmental concentrations of heavy metals and nitrogen which, together with other biomonitoring and modelling data, can be used for indicating deposition to terrestrial ecosystems and related effects across time and areas of different spatial extension.ContextFor enhancing the spatial resolution of measuring and mapping atmospheric deposition by technical devices and by modelling, moss is used complementarily as bio-monitor.AimsThis paper investigated whether nitrogen and heavy metal concentrations derived by biomonitoring of atmospheric deposition are statistically meaningful in terms of compliance with minimum sample size across several spatial levels (objective 1), whether this is also true in terms of geostatistical criteria such as spatial auto-correlation and, by this, estimated values for unsampled locations (objective 2) and whether moss indicates atmospheric deposition in a similar way as modelled deposition, tree foliage and natural surface soil at the European and country level, and whether they indicate site-specific variance due to canopy drip (objective 3).MethodsData from modelling and biomonitoring atmospheric deposition were statistically analysed by means of minimum sample size calculation, by geostatistics as well as by bivariate correlation analyses and by multivariate correlation analyses using the Classification and Regression Tree approach and the Random Forests method.ResultsIt was found that the compliance of measurements with the minimum sample size varies by spatial scale and element measured. For unsampled locations, estimation could be derived. Statistically significant correlations between concentrations of heavy metals and nitrogen in moss and modelled atmospheric deposition, and concentrations in leaves, needles and soil were found. Significant influence of canopy drip on nitrogen concentration in moss was proven.ConclusionMoss surveys should complement modelled atmospheric deposition data as well as other biomonitoring approaches and offer a great potential for various terrestrial monitoring programmes dealing with exposure and effects.

Objective This study explores the statistical relations between the concentration of nine heavy metals (HM) (arsenic (As), cadmium (Cd), chromium (Cr), copper (Cu), mercury (Hg), nickel (Ni), lead (Pb), vanadium (V), zinc (Zn)), and nitrogen (N) in moss and potential explanatory variables (predictors) which were then used for mapping spatial patterns across Europe. Based on moss specimens collected in 2010 throughout Europe, the statistical relation between a set of potential predictors (such as the atmospheric deposition calculated by use of two chemical transport models (CTM), distance from emission sources, density of different land uses, population density, elevation, precipitation, clay content of soils) and concentrations of HMs and nitrogen (N) in moss (response variables) were evaluated by the use of Random Forests (RF) and Classification and Regression Trees (CART). Four spatial scales were regarded: Europe as a whole, ecological land classes covering Europe, single countries participating in the European Moss Survey (EMS), and moss species at sampling sites. Spatial patterns were estimated by applying a series of RF models on data on potential predictors covering Europe. Statistical values and resulting maps were used to investigate to what extent the models are specific for countries, units of the Ecological Land Classification of Europe (ELCE), and moss species. Results Land use, atmospheric deposition and distance to technical emission sources mainly influence the element concentration in moss. The explanatory power of calculated RF models varies according to elements measured in moss specimens, country, ecological land class, and moss species. Measured and predicted medians of element concentrations agree fairly well while minima and maxima show considerable differences. The European maps derived from the RF models provide smoothed surfaces of element concentrations (As, Cd, Cr, Cu, N, Ni, Pb, Hg, V, Zn), each explained by a multivariate RF model and verified by CART, and thereby more information than the dot maps depicting the spatial patterns of measured values. Conclusions RF is an eligible method identifying and ranking boundary conditions of element concentrations in moss and related mapping including the influence of the environmental factors.

Samples of Hypnum cupressiforme were collected at two types of site in forest areas: within the forest stand and within forest openings, and analyzed for N and S concentrations and δ(15)N. Mosses sampled within forest openings reflect the atmospheric N deposition; however, no influence of throughfall N deposition on the N in the moss that was sampled within the forest stand was found, nor was any influence of S deposition on the S in the moss found. For the N and S concentrations in the mosses sampled within forest openings, the within-site variability was comparable to the between-site variability, and for the δ(15)N, the within-site variability was lower than the between-site. The results showed that a short distance (

Two areas near derelict calciners in Cornwall (UK) were chosen to study the uptake of arsenic from arsenic-contaminated soil into indigenous plants (heather, Calluna vulgaris; blackberry, Rubus ulmifulmus; gorse, Ulex europaeus). With total arsenic concentrations in soil ranging from 1240 to 2860 mg kg−1 at Site 1 (Tuckingmill), no adverse effects on the growth of the plants studied were observed. Very low soil-to-plant transfer factors (0.01 to 0.03) were found although they were much higher when the extractable soil arsenic concentrations were taken into account (0.1 to 1.1). In the central dump area at Site 2 (Bissoe, 9.78% [w/w] arsenic in soil), the only plant to grow was heather, although it was severely impaired. However, heather was thriving at the edge of the dump where higher soil arsenic concentrations were found (10.32% [w/w]), indicating that arsenic is not a growth-limiting factor in itself. Soil-to-plant transfer factors in the range 2 × 10−5–9 × 10−4 confirm that arsenic is indeed effectiv...

Purpose This study aimed at investigating correlations between heavy metal concentrations in mosses and modelled deposition values as well as other site-specific and regional characteristics to determine which factors primarily affect cadmium, lead and mercury concentrations in mosses. The resulting relationships could potentially be used to enhance the spatial resolution of heavy metal deposition maps across Europe. Materials and methods Modelled heavy metal deposition data and data on the concentration of heavy metals in naturally growing mosses were integrated into a geographic information system and analysed by means of bivariate rank correlation analysis and multivariate decision trees. Modelled deposition data were validated annually with deposition measurements at up to 63 EMEP measurement stations within the European Monitoring and Evaluation Programme (EMEP), and mosses were collected at up to 7, 000 sites at 5-year intervals between 1990 and 2005. Results and discussion Moderate to high correlations were found between cadmium and lead concentrations in mosses and modelled atmospheric deposition of these metals: Spearman rank correlation coefficients were between 0.62 and 0.67, and 0.67 and 0.73 for cadmium and lead, respectively (p

In the frame of the international SOILSAMP project, funded and coordinated by the Italian Environmental Protection Agency, an agricultural area was established as a reference site suitable for performing soil sampling inter-comparison exercises. The reference site was characterized for trace element content in soil, in terms of the spatial and temporal variability of their mass fraction. Considering that the behaviour of long-lived radionuclides in soil can be expected to be similar to that of some stable trace elements and that the distribution of these trace elements in soil can simulate the distribution of radionuclides, the reference site characterised in term of trace elements, can be also used to compare the soil sampling strategies developed for radionuclide investigations.

Phytoremediation is an emerging technology that employs the use of higher plants for the clean-up of contaminated environments. Progress in the field is however handicapped by limited knowledge of the biological processes involved in plant metal uptake, translocation, tolerance and plant–microbe–soil interactions; therefore a better understanding of the basic biological mechanisms involved in plant/microbe/soil/contaminant interactions would allow further optimization of phytoremediation technologies. In view of the needs of global environmental protection, it is important that in phytoremediation and plant biology studies the analytical procedures for elemental determination in plant tissues and soil should be fast and cheap, with simple sample preparation, and of adequate accuracy and reproducibility. The aim of this study was therefore to present the main characteristics, sample preparation protocols and applications of X-ray fluorescence-based analytical techniques (energy dispersive X-ray fluorescence spectrometry—EDXRF, total reflection X-ray fluorescence spectrometry—TXRF and micro-proton induced X-ray emission—micro-PIXE). Element concentrations in plant leaves from metal polluted and non-polluted sites, as well as standard reference materials, were analyzed by the mentioned techniques, and additionally by instrumental neutron activation analysis (INAA) and atomic absorption spectrometry (AAS). The results were compared and critically evaluated in order to assess the performance and capability of X-ray fluorescence-based techniques in phytoremediation and plant biology studies. It is the EDXRF, which is recommended as suitable to be used in the analyses of a large number of samples, because it is multi-elemental, requires only simple preparation of sample material, and it is analytically comparable to the most frequently used instrumental chemical techniques. The TXRF is compatible to FAAS in sample preparation, but relative to AAS it is fast, sensitive and multi-elemental. The micro-PIXE technique requires rather expensive instrumentation, but offers multi-elemental analysis on the tissue and cellular level.

In der Fachliteratur zur Bioindikation werden Hypothesen diskutiert, welche Faktoren die Metallakkumulation von Moosen neben der atmospharischen Deposition beeinflussen. Jedoch ist keine statitische Analyse bekannt, die diese Hypothesen mit grosen und einheitlich erhobenen Datensatzen uberpruft. Deshalb wird untersucht, ob Standortmerkmale wie Hohe uber NN, Meeresnahe, Kronentraufeffekt, Niederschlag, Moosart oder unterschiedliche Analyseverfahren statistisch relevanten Einfluss auf die Ergebnisse des Moos-Monitorings haben. Grundlage sind Messdaten der UNECE Heavy Metals in Mosses Surveys, Probenentnahmeorte beschreibende Metadaten sowie Flachendaten zu Niederschlag, Hohe und Landnutzung Deutschlands. Ob ein statistisch signifikanter Unterschied zwischen den Metallgehalten in Abhangigkeit von der Hohe der Probenentnahmeorte uber NN, ihrer Meeresnahe sowie ihrer Lage diesseits und jenseits von Staatengrenzen besteht, wird mit dem U-Test gepruft. Mit Spearman-Rangkorrelationsanalysen werden die statistischen Zusammenhange zwischen Metallakkumulation und Meeresnahe sowie Hohenlage uber NN quantifiziert. Neben den bivariaten Analysen wird Classification and Regression Trees (CART) angewendet, um aus der Gesamtmenge der vorliegenden Pradiktorvariablen diejenigen Faktoren zu bestimmen, die den grosten Einfluss auf die Metallbioakkumulation haben. Die Ergebnisse der statistischen Analysen werden mit entsprechenden Erkenntnissen aus der internationalen Fachliteratur abgeglichen. Es zeigt sich, dass vor allem die Moosart, der Kronentraufeffekt und der Niederschlag die Metallakkumulation in den Moosen beeinflussen. Diese Faktoren korrelieren starker mit der Metallbioakkumulation als die Quellen-bezogenen Pradiktoren wie Verkehr- und Siedlungsflachen. Die statistische Analyse des Einflusses standortlicher Randfaktoren auf die Metallbioakkumulation anhand flachendeckend vorliegender Mess- und Metadaten und Flacheninformationen zu Niederschlag, Hohe und Landnutzung ist die erste ihrer Art weltweit. Die entsprechenden Ergebnisse spiegeln den internationalen Forschungsstand weitestgehend wider, doch sind zu deren Verdichtung weitere statistische Analysen mit anderen nationalen Datenbestanden notwendig. Auch sollten im Sinne einer Sensivitatsanalyse alternative Entscheidungsbaumverfahren eingesetzt und deren Ergebnisse verglichen werden. Da die Randbedingungen der Datengewinnung von der Probenentnahme bis zur statistischen Analyse europaweit nicht vollig identisch sein konnen, mussen nicht nur die Messdaten, sondern auch — wie in Deutschland seit der Kampagne 2000 — geeignete Metadaten zum Datenerzeugungsprozess in Datenbanken dokumentiert und zusammen mit den Messdaten ausgewertet werden. Die Moosmonitoring-Verfahrensrichtlinie sollte uberarbeitet werden, um die aufgezeigten Einflusse emzuschranken, die Verfahrensstandardisierung voranzutreiben sowie die Qualitatskontrolle zu effektivieren. Hierzu sollte es gehoren, dass die Informationen zu den Moosprobenentnahmestandorten integraler Bestandteil der Datenauswertung werden. Grundsatzlich bedarf es einer statistisch fundierten Grundlagenstudie, in der die Hypothese artspezifischer Stoffakkumulation in Moosen uberpruft wird. Sollte die hier vorgestellte Datenauswertung mit den Ergebnissen der Messkampagne 2005 dieselben Resultate liefern, sollten nach Naturraumen differenzierte Korrekturfaktoren fur den Traufeinfluss, die regional unterschiedlichen Niederschlagsverhaltnisse und die Moosart auf die Metallgehalte in den Moosen angewendet werden.

The uptake and metabolism of arsenate, As(V), as a function of time and concentration were examined in the lichen Hypogymnia physodes (L.) Nyl. Lichen thalli were exposed to As(V) in the form of a solution. Exponential uptake of As(V) from 4 μg mL −1 As(V) solution was accompanied by constant arsenite, As(III), excretion back into the solution. Arsenate taken up into the lichens from 0, 0.1, 1, 10 μg mL −1 As(V) solutions was partially transformed into As(III), dimethylarsinic acid (DMA) and (mono)methylarsonic acid (MA). 48 h after exposure, the main arsenic compound in the lichens was DMA in 0.1, As(III) in 1 and As(V) in 10 μg mL −1 treatment. The proportion of methylated arsenic compounds decreased with increasing arsenate concentration in the exposure solution. These results suggest that at least two types of As(V) detoxification exist in lichens; arsenite excretion and methylation.

Micro-PIXE was applied in the study of arsenic metabolism in the lichen Hypogymnia physodes (L.) Nyl. Lichen thalli were laboratory exposed to a solution of an inorganic arsenic compound arsenate and to a control solution. Perpendicular sections that reveal the morphological properties of the lichen thallus were subjected to microbeam measurements to obtain data on the localization of arsenic and its influence on the distribution and concentrations of the selected macro- and microelements P, S, K, Ca, Cl, Mn, Fe and Zn. Five groups of elements were distinguished regarding losses and redistribution due to arsenic exposure: (1) K and Ca were depleted from all lichen layers; (2) Mn was depleted from the algal layer and lower cortex, (3) Fe was decreased in the algal layer and increased in the lower cortex, (4) Zn was decreased both in the algal layer and the medulla, but increased in the lower cortex, and (5) P and S were decreased in the medulla, but increased in the algal layer and the lower cortex.

The total activity of

For analysing element input into ecosystems and associated risks due to atmospheric deposition, element concentrations in moss provide complementary and time-integrated data at high spatial resolution every 5 years since 1990. The paper reviews (1) minimum sample sizes needed for reliable, statistical estimation of mean values at four different spatial scales (European and national level as well as landscape-specific level covering Europe and single countries); (2) trends of heavy metal (HM) and nitrogen (N) concentrations in moss in Europe (19902010); (3) correlations between concentrations of HM in moss and soil specimens collected across Norway (19902010); and (4) canopy drip-induced site-specific variation of N concentration in moss sampled in seven European countries (19902013). While the minimum sample sizes on the European and national level were achieved without exception, for some ecological land classes and elements, the coverage with sampling sites should be improved. The decline in emission and subsequent atmospheric deposition of HM across Europe has resulted in decreasing HM concentrations in moss between 1990 and 2010. In contrast, hardly any changes were observed for N in moss between 2005, when N was included into the survey for the first time, and 2010. In Norway, both, the moss and the soil survey data sets, were correlated, indicating a decrease of HM concentrations in moss and soil. At the site level, the average N deposition inside of forests was almost three times higher than the average N deposition outside of forests. © 2016, Springer-Verlag Berlin Heidelberg.

The United Nations Environment Programme (UNEP) performed field surveys at 15 sites in Bosnia–Herzegovina where depleted uranium (DU) ammunition was used by the North Atlantic Treaty Organization (NATO) during the Balkans conflict (1994–1995). During the field missions, the Italian Environmental Protection Agency (APAT) evaluated airborne contamination due to DU dusts or aerosol particles, generated at the time of the conflict by the impact of DU ammunition on hard “targets,” using lichens and tree barks as biomonitors. Each sample was analyzed by alpha-spectrometry for DU determination. The 234U/238U activity concentration ratios were used to distinguish natural from anthropogenic uranium. This paper reports the data obtained by the UNEP investigation, including (non-radioactive) metal and other element concentrations in lichen and tree bark samples measured by instrumental neutron activation analysis (INAA). The results indicated: (i) lichens and tree barks are sensitive bio-accumulators of past airborne contamination by depleted uranium dusts; (ii) 8 years after the conflict, environmental DU contamination is still present at some of the target sites; and (iii) the highest concentrations of most non-radioactive elements were found at sites used for ammunition destruction.

Lichens, sampled around Chernobyl in 1990 and in Slovenia in 1992, were analyzed for radionuclides and elements, including Cs. Data were processed by Monte Carlo aided Target Transformation Factor (MCTTFA). The resulting factors indicate environmental accumulation routes. 40K : K and 210Pb : Pb ratios tested the procedure, showing fully mixed 40K and K, while for 210Pb and Pb the expected variability in specific radioactivity was confirmed. 137Cs showed a large factor-specific variability in 137Cs : Cs ratios. For the 1990 data, MCTTFA singled-out 137Cs in a separate factor, suggesting that the overall behavior of 137Cs cannot be derived from that of Cs: source (route)-related specific radioactivity makes that all individual transport-components should be taken into account.

Adsorption of fine suspended material on the surface of aquatic plants may lead to great problems in the interpretation of results for their trace element composition, since it is quite impossible to clean the inorganic material from the biota completely. A carefully designed field experiment was performed in the River Stella in North-Eastern Italy aimed at studying the adsorption of fine suspended material on benthic algae-periphyton. More than 20 elements, were determined in water, suspended material and biota using k0-INAA, and enrichment factors were calculated for selected elements using Sc as a normalizing element.

In three Alpine lakes (Jezero na Planini pri Jezeru, Krnsko jezero and in Jezero v Ledvicah) the distribution of some metals and trace elements was determined in sediment cores using multielemental instrumental neutron activation analysis. Sediments were analysed to depths of 32 cm, 19 cm and 16 cm, respectively. Dating of sediments was done on the basis of 210Pb measurements. It was found that the levels of rare earth elements and some other lithophilic elements such as Sc, Cr, Th and U in Krnsko jezero were significantly lower than those found in the other two investigated lakes. In all three lakes changes with depth were noticed for practically all anthropogenic elements, namely As, Br, Cd, Hg, Mo and Zn. Three periods of lake history can be distinguished which reflect industrial activities in the 19th and 20th century. In the sediment profile of lake Krnsko jezero three well expressed lows of all investigated elements were found at depths of 3-3.5 cm, 6-6.5 cm and 8 cm which can be linked to two earthquakes in 1976 and 1942 and the First World War. The influence of earthquakes on the distribution of trace elements in the other two lakes was less evident. doi:10.5474/geologija.2002.040 408 Zvonka Jeran, Radojko Ja}imovi}, Polona Vre~a & Anton Brancelj

In this work an attempt to combine the results of lichen mapping with the quantitative levels of certain trace elements in Hypogymnia physodes (L.) Nyl. collected on a national scale is presented. An Index of Atmospheric Purity (IAP) was calculated using a simple method of mapping lichens based on the assessment of the cover and frequency of crustose, foliose and fruticose lichens on different tree species. For determination of trace elements in lichens k0-instrumental neutron activation analysis was used. From the IAP results it can be concluded that the epiphytic lichen flora look quite poor with more than 70% of the territory in the fourth and third classes, which represent highly polluted and moderately polluted air. By comparing IAP results with elemental levels in H. physodes using multivariate statistical methods it was found that the elemental levels do not have a direct negative effect on the diversity of lichens but can help in identification of the type of possible pollution sources and their origin.

Suspended particle adhesion on aquatic biota can significantly increase the apparent concentration of radionuclides above their endogenous value, leading to an overestimation of the uptake rate and concentration ratios. This study is an attempt to assess quantitatively the importance of suspended particle adhesion on periphyton samples (biological material coating submerged surfaces). The concentrations of 137Cs and stable Cs (133Cs) in periphyton, suspended particles and filtered water were measured to determine the net water-to-periphyton concentration ratios for 137Cs and stable Cs. The net amount of 133Cs (or 137Cs) taken up by periphyton was calculated by subtracting from the total amount of 133Cs (or 137Cs) on the collected material (periphyton+inorganic particles), the 133Cs (or 137Cs) due to the inorganic particles adhering to periphyton. The mass of suspended particles adhering to the periphyton surface was calculated using scandium as an indicator of the mineral fraction of the suspended particles. The relationship between the concentration ratios for 137Cs and stable Cs and suspended particle adhesion on periphyton external surfaces is discussed.

Aquarium experiments were performed to quantify the inorganic fraction of suspended particles deposited on the external surface of aquatic biota. The mass of suspended particles retained on the surfaces of microalgae growing on submerged substrates and the algal biomass were determined by comparing the scandium content of suspended material with that in algal communities. Scandium, a predominantly soil-associated trace element, has been used as a ‘tracer’ for the inorganic component of suspended particles, because this element is geologically ubiquitous in soils, and it is recognized that it cannot cross natural membranes of plants and other organisms. The algal biomass determined using the scandium content was compared with biomass values calculated using phytopigments as estimates of periphyton biomass. The results indicate that the suspended particle mass adhering to the external periphyton surface may accounted for up to 55% of the total mass collected on submerged artificial substrates.

The concentrations of some essential (Cu, Zn, Se) and some toxicelements (Hg, As) were determined in tissues (liver, kidneys, integument, and muscle) of the endemic cave salamander, Proteus anguinus Laurenti 1768 and Proteus anguinus parkelj ssp.n. captured in the Planina Cave, Kompolje Cave, and Jelsevnik, all situated within the Dinaric Karst in Slovenia. The highest amounts of selenium and mercury were found in the liver of Proteus anguinus specimens from all three localities. Some of the animals from the Planina Cave showed higher concentrations of copper in the liver and muscle. Pigmented subspecies of Proteus from Jelsevnik showedincreased values of arsenic in the integument and of zinc in theliver and integument. The liver of the animals contained the highest amounts of the metals analysed and therefore may be considered as a target organ. Metal levels were also measured inthe cave water and sediments. The waters were not polluted withmetals. However, the metals were relatively high in the sediments, but not to levels considered contaminated. In additionto our study of metal concentrations in Proteus tissues andhabitats, several water quality parameters were measured in the water of each locality. The main differences between the threelocalities concerned dissolved oxygen concentration and saturation, while all other physical and chemical parameterswere characteristic of the aquatic environment in the calcareousKarst region.

Samples of the moss Hypnum cupressiforme were collected at 103 locations in forests of Slovenia. At each location, samples were taken at two types of sites: under tree canopies and in adjacent forest openings. The results show that the moss collected in the forest openings reflects the surrounding land-use characteristics and, consequently, the main N emission sources. For moss sampled under canopies, the characteristics of the forest at the moss-sampling locations are more important than the main emission sources outside the forest. A regression model was used to provide the nitrogen (N) concentration in moss from the forest openings in relation to the N concentration in moss under canopies and other environmental variables. The spatial distribution of the locations of the N concentrations and δ15N values in moss collected in the forest openings and under the canopies in relation to main N deposition sources is discussed.

The retention of suspended particles transported by river flow on surfaces of freshwater plants is a potentially important process in the contamination of aquatic biota. Field experiments have been performed to test the role of benthic algae (periphyton) in trapping inorganic suspended solids transported by the river water and to discriminate between the caesium content of periphyton caused by the adherence of inorganic solids and by the active uptake inside the organisms. The contribution of caesium of suspended solids adhering to biotic surfaces was estimated by determining the scandium content (scandium method). The scandium method was used because this element is geologically ubiquitous in soils and it is not taken up actively by plants and other organisms. The mass of suspended particles retained on the surfaces of microorganisms growing on submerged substrates were determined by comparing the scandium content of suspended material with that in algal communities. Neutron activation analysis was used as the analytical method for determination for both scandium, and caesium. The results indicate that the suspended particle fraction can contribute up to 80% of the caesium contamination of periphyton samples. Active caesium uptake and accumulation by aquatic biota represents the remaining 20% of the total caesium contamination.

Natural gas contains various forms of inorganic and organic Hg species. In order to control and improve the efficiency of an industrial facility for mercury removal from natural gas at the INA-Naftaplin gas treatment plant, Molve, Croatia, a comprehensive environmental monitoring program, including mercury measurement in air, was established. Generally, total mercury concentrations in air are very low (e.g. below 10 ng.m-3) and therefore potentially subject to analytical errors (e.g. contamination). In order to control Hg contamination in air, a cost effective method, based on biomonitoring using in-situ lichen species and/or transplanted lichens specie Hypogymnia physodes was developed and optimised in recent years. The present work represents further refinement of the methodology including normalisation to geochemical background. In the present study two geographical areas were studied: (a) the INA Naftaplin Gas Treatment Plants in Croatia, where the efficiency of an industrial facility for removal of Hg from natural gas was investigated, and (b) the mercury mining area, Idrija, Slovenia. The lichen Hypogymnia physodes from a pristine area was transplanted to representative locations presented for periods of 3, 6 and 12 months during 2000/2003. In addition soil samples were collected at all sampling locations for geochemical and calculation of enrichment factors. Samples of soil samples were prepared according to standard procedures for determination of trace and major elements in soil. Determination of total mercury was performed by cold vapour atomic absorption CV AAS and MeHg by extraction/ethylation/chromatographic separation and detection by CV AFS, while other elements were performed by the instrumental neutron activation analysis INAA. The results shawed that the concentration levels of practically all elements are increased with time. These increases are mainly connected with a deposition of local soil dust, which is confirmed with the normalization of the original data for transplanted lichens with Sc. The elements that can be directly associated with the natural gas pumping and processing facilities are Hg, Ba and Br. An estimate was made for the average concentrations of Hg in the air, which was considerably elevated at stations close to technological setting for natural gas tretament, particularly during the exposure period from 6 to 12 months. The approach was validated by in Idrija with continuous monitoring of Hg in air as well as in lichens. Apart from Hg some other elements were closely evaluated. A number of elements that showed an increased enrichment in lichens are those probably associated with agricultural activity (Cu, Pb, Zn) as well as engine exhausts (Pb, Sb, Ni) or smelting and burning of fossil fuels (Sr, Zn).

Three watersheds were studied by sampling bulk precipitation deposition, seepage water at 50 cm soil depth and spring water. As the main analytical method for determination of trace elements and heavy metals in water samples, thek0-based method of INAA was used. The results showed an increased content and concentration range of trace elements in precipitation, soil water and spring water in the vicinity of the Sostanj Thermal Power Plant. We demonstrated that thek0-based method of INAA as a multielement nondestructive technique is a highly suitable approach to determining some toxic trace elements in environmental studies of the water cycle.

Previous analyses at the European scale have shown that cadmium and lead concentrations in mosses are primarily determined by the total deposition of these metals. Further analyses in the current study show that Spearman rank correlations between the concentration in mosses and the deposition modelled by the European Monitoring and Evaluation Programme (EMEP) are country and metal-specific. Significant positive correlations were found for about two thirds or more of the participating countries in 1990, 1995, 2000 and 2005 (except for Cd in 1990). Correlations were often not significant and sometimes negative in countries where mosses were only sampled in a relatively small number of EMEP grids. Correlations frequently improved when only data for EMEP grids with at least three moss sampling sites per grid were included. It was concluded that spatial patterns and temporal trends agree reasonably well between lead and cadmium concentrations in mosses and modelled atmospheric deposition.

In 2005/6, nearly 3000 moss samples from (semi-)natural location across 16 European countries were collected for nitrogen analysis. The lowest total nitrogen concentrations in mosses (

In this study, the indicative value of mosses as biomonitors of atmospheric nitrogen (N) depositions and air concentrations on the one hand and site-specific and regional factors which explain best the total N concentration in mosses on the other hand were investigated for the first time at a European scale using correlation analyses. The analyses included data from mosses collected from 2781 sites across Europe within the framework of the European moss survey 2005/6, which was coordinated by the International Cooperative Programme on Effects of Air Pollution on Natural Vegetation and Crops (ICP Vegetation). Modelled atmospheric N deposition and air concentration data were calculated using the Unified EMEP Model of the European Monitoring and Evaluation Programme (EMEP) of the Convention on Long-range Transboundary Air Pollution (CLRTAP). The modelled deposition and concentration data encompass various N compounds. In order to assess the correlations between moss tissue total N concentrations and the chosen predictors, Spearman rank correlation analysis and Classification and Regression Trees (CART) were applied. The Spearman rank correlation analysis showed that the total N concentration in mosses and modelled N depositions and air concentrations are significantly correlated (0.53 ≤ rs ≤ 0.68, p < 0.001). Correlations with other predictors were lower than 0.55. The CART analysis indicated that the variation in the total N concentration in mosses was best explained by the variation in NH4+ concentrations in air, followed by NO2 concentrations in air, sampled moss species and total dry N deposition. The total N concentrations in mosses mirror land use-related atmospheric concentrations and depositions of N across Europe. In addition to already proven associations to measured N deposition on a local scale the study at hand gives a scientific prove on the association of N concentration in mosses and modelled deposition at the European scale.

In recent decades, mosses have been used successfully as biomonitors of atmospheric deposition of heavy metals. Since 1990, the European moss survey has been repeated at five-yearly intervals. Although spatial patterns were metal-specific, in 2005 the lowest concentrations of metals in mosses were generally found in Scandinavia, the Baltic States and northern parts of the UK ; the highest concentrations were generally found in Belgium and south-eastern Europe. The recent decline in emission and subsequent deposition of heavy metals across Europe has resulted in a decrease in the heavy metal concentration in mosses for the majority of metals. Since 1990, the concentration in mosses has declined the most for arsenic, cadmium, iron, lead and vanadium (52e72%), followed by copper, nickel and zinc (20e30%), with no significant reduction being observed for mercury (12% since 1995) and chromium (2%). However, temporal trends were country-specific with sometimes increases being found.

The study was focused on understanding the mercury contamination caused by a cement plant. Active and passive biomonitoring with epiphytic lichens was combined with other instrumental measurements of mercury emissions, mercury concentrations in raw materials, elemental mercury concentrations in air, quantities of dust deposits, temperatures, precipitation and other measurements from the cement plant’s regular monitoring programme. Active biomonitoring with transplanted lichens Pseudevernia furfuracea (L.) Zopf was performed at seven of the most representative sites around the cement plant and one distant reference site for periods of 3, 6 and 12 months. In situ lichens of different species were collected at the beginning of the monitoring period at the same sites. Mercury speciation of the plant exhaust gas showed that the main form of emitted mercury is reactive gaseous mercury Hg2 + , which is specific for cement plants. Elemental mercury in air was measured in different meteorological conditions using a portable mercury detector. Concentrations in air were relatively low (on average below 10 ng m − 3). In situ lichens showed Hg concentrations comparable to lichens taken from the background area for transplantation, indicating that the local pollution is not severe. Transplanted lichens showed an increase of mercury, especially at one site near the cement plant. A correlation between precipitation and Hg uptake was not found probably due to a rather uniform rainfall in individual periods. Dust deposits did not influence Hg uptake significantly. Lichens vitality was affected over longer biomonitoring periods, probably due to some elements in dust particles, their alkalinity and the influence of other emissions. Mercury uptake measured in vital transplanted lichens was in a good correlation with the working hours (i.e. emitted Hg quantity) of the kiln. The study showed that selected lichens could be used to detect low to moderate Hg emissions from a cement plant and that the biomonitoring procedure could be further standardized and used as part of an environmental monitoring programme.

Thalli of epiphytic lichen Hypogymnia physodes (L.) Nyl. and terricolous Cladonia furcata (Huds.) Schrad., collected from an area with background arsenic concentrations, were exposed to 0, 0.1, 1 and 10 microg mL(-1) arsenate (As(V)) solutions for 24 h. After exposure they were kept in the metabolically active state for 0, 24 and 48 h in a growth chamber. In the freeze dried samples glutathione (GSH), glutathione disulphide (GSSG), cysteine (Cys) and cystine were analysed and induction of phytochelatin (PC) synthesis measured by reversed-phase high-performance liquid chromatography in combination with fluorescence detection or UV spectrometry. Total arsenic content in thalli was measured by instrumental neutron activation analysis (INAA). In H. physodes, which contained higher amounts of arsenic compared to C. furcata, total glutathione content significantly decreased in samples exposed to 10 microg mL(-1) As(V), whereas in C. furcata a significant increase was observed. In both species PC synthesis was induced in thalli exposed to 10 microg mL(-1).

The aim of this study was, for the first time ever, to thoroughly identify the factors influencing Cd, Hg and Pb concentrations in mosses sampled within the framework of the European Heavy Metals in Mosses Surveys 1990–2005. These investigations can be seen as a follow up of a previous study where only the moss data recorded in the survey 2005 was included in the analysis (Schroder et al. 2010). The analyses of this investigation give a complete overview on the statistical association of Cd, Hg and Pb concentrations in mosses and sampling site-specific and regional characteristics, encompassing data from 4661 (1990), 7301 (1995), 6764 (2000) and 5600 (2005) sampling sites across Europe. From the many metals monitored in the European moss surveys, Cd, Hg and Pb were used as examples, since only for these three metals deposition measurements are being recorded in the framework of the European Monitoring and Evaluation Programme (EMEP). As exemplary case studies revealed that other factors besides atmospheric deposition of metals influence the element concentrations in mosses, the moss datasets of the above mentioned surveys were analysed by means of bivariate statistics and decision tree analysis in order to identify factors influencing metal bioaccumulation. In the analyses we used the metadata recorded during the sampling as well as additional geodata on, e.g., depositions, emissions and land use. Bivariate Spearman correlation analyses showed the highest correlations between Cd and Pb concentrations in mosses and EMEP modelled total deposition data (0.62 ≤ rs ≤ 0.73). For Hg the correlations with all the tested factors were considerably lower (e.g. total deposition r s ≤ 0.24). Decision tree analyses by means of Classification and Regression Trees (CART) identified the total deposition as the statistically most significant factor for the Cd and Pb concentrations in the mosses in all four monitoring campaigns. For Hg, the most significant factor in 1990 as identified by CART was the distance to the nearest Hg source recorded in the European Pollutant Emission Register, in 1995 and 2000 it was the analytical method, and in 2005 it was the sampled moss species. The strong correlations between the Cd and Pb concentrations in the mosses and the total deposition can be used to calculate deposition maps with a regression kriging approach on the basis of surface maps on the element concentrations in the mosses.

This paper aims to quantify the soil sampling uncertainty arising from the short-range spatial variability of elemental concentrations in the topsoils of agricultural, semi-natural, and contaminated environments. For the agricultural site, the relative standard sampling uncertainty ranges between 1% and 5.5%. For the semi-natural area, the sampling uncertainties are 2–4 times larger than in the agricultural area. The contaminated site exhibited significant short-range spatial variability in elemental composition, which resulted in sampling uncertainties of 20–30%.

This study aimed at cross-border mapping metal loads in mosses in eight European countries in 1990, 1995, and 2000 and at investigating confounding factors. Geostatistics was used for mapping, indicating high local variances but clear spatial autocorrelations. Inference statistics identified differences of metal concentrations in mosses on both sides of the national borders. However, geostatistical analyses did not ascertain discontinuities of metal concentrations in mosses at national borders due to sample analysis in different laboratories applying a range of analytical techniques. Applying Classification and Regression Trees (CART) to the German moss data as an example, the local variation in metal concentrations in mosses were proved to depend mostly on different moss species, potential local emission sources, canopy drip and precipitation.

In the frame of the international SOILSAMP project, funded and coordinated by the National Environmental Protection Agency of Italy (APAT), uncertainties due to field soil sampling were assessed. Three different sampling devices were applied in an agricultural area using the same sampling protocol. Cr, Sc and Zn mass fractions in the collected soil samples were measured by k 0 -instrumental neutron activation analysis (k 0 -INAA). For each element-device combination the experimental variograms were calculated using geostatistical tools. The variogram parameters were used to estimate the standard uncertainty arising from sampling. The sampling component represents the dominant contribution of the measurement uncertainty with a sampling uncertainty to measurement uncertainty ratio ranging between 0.6 and 0.9. The approach based on the use of variogram parameters leads to uncertainty values of the sampling component in agreement with those estimated by replicate sampling approach.

Two country-wide surveys using epiphytic lichens as biomonitors of atmospheric pollution carried out during 2000 and 2001 in Slovenia were compared with surveys in 1991 and 1992. In the first survey, epiphytic lichen cover was studied in more than 500 plots of the 4 x 4 km national grid carried out within the framework of forest decline inventories. In the second survey, the epiphytic lichen Hypogymnia physodes (L.) Nyl., was collected on a 16 x 16 km bioindication grid and analysed for S, N, As, Br, Ce, Cd, Cr, K, La, Mo, Rb, Sb, Th, U and Zn contents. Only 'forested area' sampling points were included in the present study. Lichen cover was low, with about 70% of plots with less than 10% foliose lichen cover. No relationship was found between Hypogymnia trace element, N and S concentrations and foliose epiphytic lichen cover.

Different extraction procedures were applied to improve the extraction efficiency of arsenic compounds from lichens. Two lichen species were chosen from an arsenic-contaminated environment: epiphytic Hypogymnia physodes (L.) Nyl. and terricolous Cladonia rei Schaer. Samples were extracted with water at temperatures of 20, 60 and 90 °C, using mixtures of methanol/water (9:1, 1:1 and 1:9), Tris buffer and acetone and the extracts speciated. Water and Tris buffer showed the best extraction efficiency of all extractants used; however, the extraction efficiency was still less than 23%. Since a major fraction of arsenic appeared to be associated with trapped soil particles, a sequential extraction procedure originally designed for soils (extraction steps: (1) 0.05 mol l −1 (NH 4 ) 2 SO 4 ; (2) 0.05 mol l −1 (NH) 4 H 2 PO 4 ; (3) 0.2 mol l −1 NH 4 -oxalate buffer, pH 3.25; (4) mixture of 0.2 mol l −1 NH 4 -oxalate buffer and 0.1 mol l −1 ascorbic acid, pH 3.25; (5) 0.5 mol l −1 KOH) was applied and found to remove 45% of the total arsenic from H. physodes and 83% from C. rei . The lipid-soluble fraction of arsenic was estimated by k 0 -INAA analysis of diethylether extracts and was found to be negligible. An HPLC-UV-HGAFS system was used to determine the arsenic compounds extracted. In both lichen species, arsenous acid, arsenic acid, monomethylarsonic acid, dimethylarsinic acid, arsenobetaine, trimethylarsine oxide and glycerol-ribose were detected. In addition, phosphate-ribose was found in H. physodes .

This paper describes the use of epiphytic lichens as bioindicators for spatial monitoring of mercury and other elements in air near the natural gas treatment facilities at Molve, Croatia. It is well known that at this location the concentration of mercury in natural gas is very high and therefore it has to be removed from natural gas before further processing in order to prevent technological and environmental problems. In order to monitor the efficiency of an industrial facility for removal of mercury from natural gas, mercury measurements in air and lichens were performed during 9 months in 1997/1998. In situ lichens Parmelia sulcata, Xantoria parientina and Hypogymnia physodes and transplanted lichen species Hypogymnia physodes were used. A good correlation between mercury concentrations in air and lichens was found. The concentrations of barium and bromium were also significantly elevated in transplanted lichens, most probably related to technological process at the gas treatment plant and/or other geological factors. It was confirmed that lichens can successfully be used as bioindicators, provided a careful experiment is designed, particularly the amount of lichens transplanted, the duration of exposure and the initial levels and homogeneity of transplanted lichens.

In 1992, a monitoring survey has been started on the national scale in Slovenia using the epiphytic lichen Hypogymnia physodes (L.) Nyl. The primary aim has been to analyse lichens using the k(0)-based INAA method to obtain information about the levels of elements in the atmosphere and to identify significant pollution sources. Monte Carlo-Assisted Factor Analysis was applied to a data set of the 28 elements As, Ag, Ba, Br, Ce, Cd, Co, Cr, Cs, Fe, Ga, Hf, Hg, K, La, Mo, Na, Rb, Sb, Sc, Se, Sr, Sm, Tb, Th, U, W and Zn, which have been selected from the elements determined as the most important ones for the identification of pollution sources. A Monte Carlo approach has been used to give more insight into the uncertainties and significance levels of the factor analysis results. It has been found that concentration patterns in lichens yielded 9 factors (source types) which are presented and discussed in detail. The geographical patterns of the contributions of all factors are also shown.