ࡱ>  )bjbj s0~M ((((($LLLP0Lhi*hhhhhhh$kDnAh(Ah((4"i @ @ @"((h @h @ @N%^a i@.Z _0h8i0hi_n8n`aa"n(aP @AhAhj<hin :CHANGES OF Ba CONTENTS IN SEDIMENTS OF KUPA RIVER (CROATIA) 15 YEARS AFTER DISCOVERY OF Ba ANOMALY COMPLEMENTED BY SEQUENTIAL EXTRACTION Dr. Stanislav Fran iakovi-Bilinski1 Dr. Halka Bilinski1 Dr. Sanja Sakan2 Dr. Dragana orevi2 Prof. Dr. Aleksandar Popovi3 1 Ruer Boakovi Institute, Division for Marine and Environmental Research, POB 180, HR-10002 Zagreb, Croatia 2 Centre of Excellence in Environmental Chemistry and Engineering  ICTM, University of Belgrade, Njegoaeva 12, Belgrade 11158, Serbia 3 Faculty of Chemistry, University of Belgrade, Studentski trg 12-16, Belgrade 11000, Serbia ABSTRACT The Kupa River, located in the west-central part of Croatia, is a 294 km long tributary of the Sava River, belonging to the Danube watershed. An extreme barium anomaly in sediments of Kupica and Kupa rivers was discovered during 2003 by Fran iakovi-Bilinski. It originates from an abundant barite mine in Homer-Lokve area, from where it penetrated to Kupica River source. From there the Ba-anomaly in sediments was followed more than 120 km downstream along both rivers. This discovery has a big potential to be used in future sediment transport studies in rivers. Therefore, we repeated sampling on most important locations in 2018, exactly 15 years since the anomaly discovery. The sequential extraction procedure of the EC Bureau of Reference was applied to investigate the transport and fractionation of Ba. During mentioned period of 15 years following processes related with Ba-distribution were observed in fraction <63 m: Ba-concentrations decreased more than 10 times in Kupica River, from 5790 to 385 mg/kg at Brod na Kupi and 473 mg/kg at Ievnica near the Kupica source. Also, at the first location in Kupa River after confluence with Kupica Ba-concentration decreased from 1070 to 429 mg/kg. This significant decrease is a consequence of abandoning of barite mine in 1994, after which self-purification process of Kupica and Kupa river sediments gradually started. Large quantities of Ba gradually shifted more downstream and in the middle course of the river Ba-deposition in sediments is still going on. At location Jurovo in the middle course of the river concentrations remained about the same in both years, while in Ozalj several km downstream concentration moderately decreased from 341 to 241 mg/kg. Very important finding is that Ba-anomaly in the time frame of 15 years arrived at least 50 km more downstream. Namely, in 2003 at location Pokupsko in the lower course of Kupa River, Ba-concentration was only 78.4 mg/kg, what is about the background level for this region. In 2018 Ba-concentrations significantly increased to 209 mg/kg. At the far end of the river course in Sisak, Ba-anomaly has not yet been observed concentrations of Ba remained almost the same (65 mg/kg in 2003 and 63.8 mg/kg in 2018). From analysis of coarser sediment fraction 63-2000 m can be concluded that barium is bound with fine particles. Results of sequential analysis showed that Ba was extracted in the following order for ( 63 m sediment fraction: reducible > residual > soluble in acid > oxidizable, while for 63-2000 m sediment fraction: reducible > soluble in acid > residual > oxidizable. The highest Ba-content was found in reducible fraction, what indicated that Fe and Mn minerals acted as natural accumulators for Ba in investigated sediments. This association indicated that Ba was potentially extractable. It could have been mobilized from the sediment into the aquatic environment due to decomposition of Fe and Mn oxides under slightly reducing conditions. Keywords: Kupa River (Croatia), barium anomaly, sediments, sequential extraction, fractionation of Ba. INTRODUCTION An extreme barium anomaly in sediments of Kupica and Kupa rivers was discovered in 2003 during work on Ph.D. Thesis of Fran iakovi-Bilinski and was published in 2006 [1]. This anomaly in Kupa River sediments was not known before. After a long and complicated search it was discovered that the source of this Ba-contamination was an abundant barite mine in Homer-Lokve area. As a result of un-careful mine waste disposal in a channel leading to an abyss, the contamination penetrated through vulnerable karstic aquifers and appeared at Kupica River source. About the same time a study on karst groundwater protection in the Kupa River catchment area and sustainable development was carried out and it pointed to extreme vulnerability of karstic aquifers around Kupa River [2]. From Kupica River source the extreme concentrations of barium in sediments were followed for more than 120 km downstream along Kupica and Kupa rivers. Our study has a big potential to be used in the future to study sediment transport processes in rivers and investigated rivers act as an excellent natural laboratory. In spite of decades of research, sediment transport, in particular in gravel-bed rivers, is still a difficult issue [3]. There are still plenty of open issues in this knowledge worldwide, also it is hard to find appropriate river to follow sediment transport processes. Therefore, we repeated sampling on several most important locations in 2018, exactly 15 years since the anomaly discovery, with the aim to see which processes happened during that time frame. Also, the sequential extraction procedure of the European Community Bureau of Reference (BCR) was applied to investigate the fractionation of Ba, especially with the aim to investigate its possible bioavailability. STUDY AREA AND SAMPLING The Kupa River basin, presented in Figure 1, occupies the west-central part of Croatia and is shared by two neighbouring countries (Slovenia, Bosnia and Herzegovina). It is the tributary of the Sava River and meets the latter at Sisak after traversing a distance of 294 km. The Sava River belongs to the Danube River watershed and enters the Danube River at Belgrade (Serbia). Kupa River and its watershed have been under intensive scientific investigations during last two decades and among other subjects geochemical assessment of its sediments [4] and fluvial geomorphology [5] were studied in details. Sampling was performed at 18 representative locations along Kupica and Kupa Rivers. Positions of sampling locations are presented in Figure 2. Two locations (I and 51) are on Kupica River, one location (52) is on Kupa River upstream Kupica inflow, while all other locations are in Kupa River downstream from Kupica River inflow. Locations where fine grained sediment accumulates along the river bank were chosen. On each sampling site, at least three grab samples of active fine-grained surface sediment (05 cm deep) were collected from different places in an area of 5 m2. From this material a composite sample was taken weighing up to 1.5 kg. This procedure decreased the possible bias caused by local variability.  Figure 1. Position of Kupa River drainage basin within Croatia and neighbouring countries.  Figure 2. Position of barite mine and of sampling stations along the Kupa River. MATERIALS AND METHODS After sampling the sediments were dried in air at room temperature and then sieved through a 2000 m and 63m sieves (Fritsch, Germany) to obtain two sediment fractions: fine fraction containing clay and silt (<63m) and coarser fraction containing sand (63-2000 m). Obtained sediment fractions were used for further analysis. Sequential extraction was performed using the optimized BCR procedure [6]. The four steps of the applied sequential extraction procedure identify four fractions (F I F IV), reflecting different degrees of elemental solubility: F I: fraction soluble in acid - metals exchangeable or associated with carbonates; F II: reducible fraction - metals associated with oxides of Fe and Mn; F III: oxidizable fraction - metals associated with organic matter and sulphides; F IV: residual fraction - metals strongly associated with the crystalline structure of minerals. The ICP/OES spectroscope iCAP-6500 Duo was used to determine the element concentrations. The sum of elemental concentration of each fraction represents total amounts of elements. Analytical data quality was controlled by using quality control methods. RESULTS AND DISCUSSION Results of sequential analysis of barium in Kupa River sediments are shown in Table 1, while downstream distribution of Ba-concentrations in sediments of Kupa River in 2003 and 2018 are shown in Figure 3. Table 1. Results of sequential analysis of barium in Kupa River sediments (mg/kg( SampleFraction Ba IBa IIBa IIIBa IVBa (Ba 2003*I`<63m44.229440.494.7473-4<63m32.667.813.012824134152<63m11.930.22.9413.658.775.22<63m32.910318.024439838638<63m31.512521.830.520978.4 D<63m35.816417.62114291070**44<63m15.136.53.808.4563.86551<63m52.426227.942.83855790I63-2000 m16.650.75.269.6582.2-463-2000 m30.961.014.6101208-5263-2000 m3.275.802.095.0516.2-263-2000 m10.414.04.7715.244.3-3863-2000 m13.235.84.065.1958.3- D63-2000 m12.831.42.527.4354.2-4463-2000 m4.747.301.131.9915.2-5163-2000 m14.236.83.579.3263.8-4563-2000 m7.4127.81.973.4140.5-563-2000 m7.775.142.213.5418.6-963-2000 m9.3715.63.244.5532.8-2863-2000 m6.089.221.272.0318.6-4163-2000 m3.494.410.921.2610.1-4963-2000 m8.5917.43.208.5537.8-2963-2000 m3.274.320.891.9710.4-3663-2000 m12.239.81.764.3658.2-*Ba concentrations in 2003 (aqua-regia extraction ICP-MS) are taken from ref. [1]. **Data from 2003 are from location }aga in Slovenia (about 5 km downstream from D, in sampling map 50), which is currently not available for sampling Therefore D was selected as closest accessible point, which could be compared with }aga location.  Figure 3. Barium concentrations in f<63 m of Kupa River sediments in years 2003 and 2018 going downstream. X-axis presents km of river flow and Y-axis presents mg/kg (ppm) of Ba. During mentioned period of 15 years following processes related with Ba-distribution were observed in fraction <63 m: Ba-concentrations decreased more than 10 times in Kupica River, which brought contamination to Kupa River. In year 2003 Ba-concentrations in Kupica River were as high as 5790 mg/kg, while in 2018 they dropped to 385 mg/kg at Brod na Kupi and 473 mg/kg at Ievnica near the Kupica source. Also at the first location in Kupa River after confluence with Kupica concentration decreased in 15 years from 1070 mg/kg to 428 mg/kg. This significant decrease in Ba-concentrations is a consequence of abandoning of barite mine in Homer in 1994, after which karstic underground was washed of Ba and gradually started self-purification process of Kupica and Kupa river sediments. Those large quantities of Ba gradually shifted more downstream and in the middle course of the river Ba-deposition in sediments is still going on. At location Jurovo in the middle course of the river concentrations remained about the same in 2003 (386 mg/kg) and in 2018 (398 mg/g), while in Ozalj several km downstream concentration moderately decreased from 341 mg/kg to 241 mg/kg. Very important finding is that Ba-anomaly in the time frame of 15 years arrived at least 50 km more downstream, as at location Pokupsko in the lower course of Kupa River in 2003 Ba-concentration was only 78.4 mg/kg, what is about the background level for this region, while in 2018 it significantly increased to 209 mg/kg. At the far end of the river course in Sisak, just before confluence with Sava, Ba-anomaly has not yet been observed, as Ba-concentrations remained almost the same (65 mg/kg in 2003 and 63.8 mg/kg in 2018). Our data are preliminary and based on limited number of locations, therefore a more detailed study should be conducted to study in details Ba transport in sediments. Also, used methods in 2003 and 2018 are not the same in 2003 aqua regia digestion was used, while in 2018 sequential extraction procedure was used. Sum of four extracted fractions was used for comparison with aqua regia results from 2003. Because of lack of fine sediment material on some locations and for some comparisons, an analysis of coarser fraction 63-2000 m was also performed. On all locations except one (sample 4 under dam of Ozalj hydropower plant) Ba-concentrations were very low in coarser fraction, from what can be concluded that barium is bound with fine particles (clay and silt). Unfortunately in 2003 coarser fraction was not analysed, therefore we dont have any data for comparison. The reason why on location 4 Ba-content in sample of sediment fraction 63-2000 m was almost as high as in fine (<63 m) fraction is its granulometric composition within coarser fraction. Unfortunately granulometric analysis was not performed, but during sampling and sample preparation it was observed that this sample was very muddy, full of clay particles. Also, within sieved coarser fraction 63-2000 m prevailed particles size of which is much closer to 63 m, than particles of larger size.  EMBED Excel.Chart.8 \s  Figure 4. Distribution of barium content by fractions. Explanation: Ba I - fraction soluble in acidmetals exchangeable or associated with carbonates; Ba II - reducible fractionmetals associated with oxides of Fe and Mn; Ba III - oxidizable fractionmetals associated with organic matter and sulfides, and Ba IV - residual fraction. Note: On left side of graphic (samples I-51) are presented samples of fine granulometric fraction (<63 m), while on right side of graphic (after brake, samples I-36) are presented samples of fraction 63 2000 m. Distribution of barium content by fractions and localities is shown on Figure 4. Percentage distribution, calculated as the average content of the extracted element in each fraction with respect to the total content of extracted element showed that barium was extracted in the following order: reducible fraction (49.20 %) > residual fraction (30.76 %) > fraction soluble in acid (14.79 %) > oxidizable fraction (6.42 %) for ( 63 m fraction and reducible fraction (48.40 %) > fraction soluble in acid (25.63 %) > residual fraction (19.00 %) > oxidizable fraction (8.48 %) for 63-2000 m fraction. Generally, barium is capable of adsorption onto clays, manganese oxides and zeolite minerals and is found to occur in deep sea manganese nodules and freshwater manganese deposits [7]. The highest content of Ba was found in reducible fraction indicated that Fe and Mn oxides acted as natural accumulators for barium in investigated sediments. This association indicated that barium was potentially extractable. It could have been mobilized from the sediment into the aquatic environment due to decomposition of Fe and Mn oxides under slightly reducing conditions. Adsorption onto metal oxides in soils and sediments probably acts as a control over the concentration of barium in natural waters, as shown in literature [8]. The significant percent of Ba associated with the reducible fraction as observed in this current study raise concerns regarding their potential mobility in the water phase and consequent bioavailability during dredging/remediation. Oxidizable fraction was the least representative, which is in accordance with results of Nogueirol and Alleoni [9]. The low contents of barium associated with F III can be due to low contents of organic matter in sediments [10]. CONCLUSION Exactly 15 years after discovery of an extreme barium anomaly in sediments of Kupica and Kupa rivers in 2003, a new research was conducted, with the aim to follow downstream transport of barium in sediments and to investigate fractionation of Ba. Kupa River has a big potential as an ideal natural laboratory to study these processes. The following conclusions were obtained within our research: During mentioned period of 15 years in fraction <63 m Ba-concentrations decreased more than 10 times in Kupica River, which brought contamination to Kupa River. Also at the first location in Kupa River after confluence with Kupica concentration significantly decreased in 15 years. This is a consequence of abandoning of barite mine in Homer in 1994, after which karstic underground was washed of Ba and gradually started self-purification process of Kupica and Kupa river sediments. Large quantities of Ba gradually shifted more downstream and in the middle course of the river Ba-deposition in sediments is still going on. Very important finding is that Ba-anomaly in the time frame of 15 years arrived at least 50 km more downstream, to location Pokupsko (sample 38) in the lower course of Kupa River. At the far end of the river course in Sisak (sample 44), just before confluence with Sava, Ba-anomaly has not yet been observed, as Ba-concentrations remained almost the same as in 2003. On all locations except one (sample 4 under dam of Ozalj hydropower plant) Ba-concentrations were very low in coarser fraction (63-2000 m), from what can be concluded that barium is bound with fine particles (clay and silt). Fractionation results suggest that an appreciable proportion of Ba may be remobilized and made readily available under slightly reducing conditions. Further research is suggested to identify either organic matter or microbes which form reducing conditions and bring Barite into soluble form. ACKNOWLEDGEMENTS We thank M.Sc. Kreimir Maldini from Hrvatske vode (Croatian water authorities) who helped us with drying and sieving of collected sediment samples. The authors are also very grateful to Sandra `krivanj for analytical results. REFERENCES [1] Fran iakovi-Bilinski S., Barium anomaly in Kupa River drainage basin, Journal of geochemical exploration, vol.  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