ࡱ> pbjbj s{{?F: : $PU*TTTTTTT$XZUU4U"...FT.T..2rJMq(!L.TU<U4Lra[."|a[\MMa[4N.UU(@Ua[: Z:MERCURY CONTENTS IN WATER, SEDIMENT AND TUFA IN KARSTIC KRKA RIVER, CROATIA Mr. }eljko Kwokal1 Dr. Stanislav Fran iakovi-Bilinski1 Dr. Neven Cukrov1 1 Ruer Boakovi Institute, Division for Marine and Environmental Research, Croatia ABSTRACT The Krka River is a pristine karstic stream and unique model system for the understanding and interpretation of environmental records in tufa precipitating rivers worldwide. The river is characterized by 7 main and numerous small tufa barriers grown in a constant and dynamic process depending upon many physicochemical factors. An evaluation of the quality status of the pristine karstic, tufa depositing aquatic environment of the Krka River National Park based on the analysis of mercury contents was performed for the first time. The aim of the study was to compare total mercury concentrations obtained in surface sediments with those in the recent tufa. Moreover, mercury concentration in tufa and sediments was compared with those in ambient water. Research was undertaken during three years, and analyses of mercury in water, sediment and tufa were conducted by cold vapor atomic absorption spectrometry (CVAAS). The concentrations of mercury in water were very low revealing a pristine aquatic environment. During the three year research period, mercury concentrations in water varied from 0.5 ngL-1 to 17 ngL-1. In the surface sediments concentrations varied from 0.01 to 0.13 mgkg-1 dry weight. Mercury concentrations in the sediment column vary from 0.07 in the deepest layer to 0.13 mgkg-1 dry weight in the surface layer, indicating a continually increasing anthropogenic pressure during the last fifty years. In recent tufa, mercury concentrations varied from 0.008 to 0.092 mgkg-1 dry weight. Box plot statistical analysis was performed, which found only one anomaly of lower degree (outlier) in sediment of location K-11. Cluster analysis of Q-mode was performed on dataset consisting of sediment and tufa data. Two clusters were obtained: Cluster 1 with mean Hg-concentration of 0.075 mgkg-1 and Cluster 2 with mean Hg concentration of 0.024 mgkg-1. It is obvious that Cluster 1 is under some anthropogenic influence, while Cluster 2 is rather clean. Majority of samples of Cluster 1 are located in area around Brljan lakes and is assumed that this Hg-contamination originates from industry and waste water of the Knin town. It seems that self-purification mechanism exists in Krka River, as elevated Hg-concentrations are not present downstream Roki slap waterfall and all samples in the downstream part of the river belong to anthropogenically clean Cluster 2. Keywords: mercury, sediments, tufa, karstic rivers, Krka, Croatia, Q-mode cluster analysis INTRODUCTION Krka is a typical groundwater-fed karstic river in Dalmatian karst that enters in the Adriatic Sea, receiving a considerable fraction of its surface water flow through subsurface groundwater discharge. Most of it derives from the Zrmanja river watershed through submerged or ephemeral springs, as well as from a diffuse recharge which is not yet localized. The hydrogeological drainage area of the Krka is around 2 427 km2 [1, 2]. The average annual river discharge at Skradinski Buk Waterfalls (end of freshwater part) in last 50 years has varied between 40 and 60 m3s-1, with a minimum flow of 5 m3s-1 and maximum of 565 m3s-1 [1, 2]. The length of the fresh-water section is 49 km, while the estuary is extended for additional 23.5 km. The canyon of the Krka River is located at the Dinaric carbonate platform, consisting of carbonate rocks, mostly limestones and dolomites. Sub-recent and recent carbonate deposits in the river consist of calcareous cascade and barrage tufa. Tufa depositing is a constant, dynamic process, involving physico-chemical factors and organisms living in the water Rogerson et al., 2008) [3, 4]. Owing to the picturesque scenery of tufa cascades stretching over tens of km, as well as its biological and geological characteristics, the lower part of the river region is protected as a National park Krka. Anthropogenic pollution of the river by ecotoxic metals and radionuclides has been identified downstream of city of Knin that is located a few km downstream of the Krka River spring [5, 6]. In the 2011 census, the population of Knin was 15 407in the city with density of 43.3 inhabitants per square kilometre. Up to now, all waste waters from the city have entered the Krka River without any pre-treatment. This considerably influences the water quality before entrance into National park Krka. However, a significant self-purification process takes place through several small cascades lakes (Manojlova ki Waterfalls) formed behind tufa barriers in the middle part of the river flow, where intensive scavenging through sedimentation and precipitation results in significant decrease of ecotoxic metal concentrations [6]. At the moment, a waste water treatment system for the city of Knin and its municipality is still under construction. The aim of the present work was to obtain mercury concentrations in the environment of the Krka River. Moreover, total mercury concentrations obtained in surface sediments was compared with those in the recent tufa and with those in river water. STUDY AREA Study area with sampling locations (Figure 1) include entire freshwater part of the Krka River and their main tributary (Kr i, Zrmanja and ikola Rivers) Kr i River and ikola River are surface tributaries, while Zrmanja River has underground inflow to the Krka River. Moreover, Kr i  and ikola rivers are without water during dry season (typically May to October), while Zrmanja have permanent flow. Krka and tributaries are tufa precipitating streams.  Figure 1. Study area with sampling locations. Grey surface presents area of National park Krka. MATERIALS AND METHODS Sampling and sample preparation Sampling was performed between November 2004 and July 2007. For Hg measurements in water, samples were collected in pre-cleaned SIMAX Sklrny Kavalier borosilicate glass reagent bottles (Szava, Czech Republic, 1 L). Bottles were cleaned with Suprapur nitric and hydrochloric acid (Merck, Germany) and rinsed with doubly deionized water. Recent tufa was collect manually with plastic spatulas at tufa barriers, while sediment samples were collected by scuba diving by hand-driven acrylic corers. Sampling sites (Fig. 1) were determined by GPS instrument Garmin GPSMap 72 (Kansas City, USA) with an accuracy of 5 m. Sediment and tufa samples were dried at room temperature until constant weight and stored in polyethylene bags. Dried samples were digested by mixture of Suprapur perchloric (1 ml) and nitric acids (10 ml) in combination with hydrofluoric acid (5-10 ml) (Merck, Darmstadt, Germany), in closed teflon crucible (35 ml volume) at temperature of ~ 180C CVAAS Hg analysis CVAAS (Cold Vapour Atomic Absorption Spectrometry) method was used for mercury measurements. This method requires conversion of all forms of mercury to Hg 2+ (acid, oxidative digestion) and its reduction to Hg0 by Sn2+ solution (10% SnCl2 in 20% H2SO4), adsorption/desorption on Au-wire and detection of Hg0 vapour by Elemental Mercury Detector (a mercury MonitorTM3200 by a Thermo Separation Products). For the total mercury measurements the soil sample were treated/decomposed in a closed quartz vessel (pressure about 3 bars) with mixture of 10 ml of nitric and perchloric acids at 140C. For each sample a known amount of standard Hg solution was subsequently added for the calibration purposes. The actual mercury concentration obtained was corrected with the average blank value of the system. The detection limit of such CVAAS system is 5 pg with the linearity range from 5 to 10 000 pg. The detection limit of the method for soil and sediment samples is 0.01 ng g-1. The reproducibility is 2% for concentrations >200 ng g-1 and 10% for concentrations >1 ngg-1. The efficiency is > 90% for solid matrices. RESULTS AND DISCUSSION Mercury concentrations in water In Table 1 are presented Hg-concentrations in water of Krka and Zrmanja rivers, measured at 14 locations on several occasions between November 2004 and July 2007. In the last column mean value for each station is presented. Measurements were not performed each time on each location, therefore full time series do not exist. Table 1. Hg concentrations (in ngL-1) measured in water of Krka and Zrmanja rivers LocationNov.04Jan.05May.05Jul.05May.06Jul.06Jul.07MeanK-011.101.050.770.49-1.100.790.88K-034.701.701.00-1.4010.001.193.33K-041.30-1.450.601.103.00-1.49K-12-----3.200.731.97ZR-1------0.390.39K-30-1.270.950.95-2.000.971.23K-311.601.200.680.51---1.00K-323.401.700.940.89---1.73K-334.201.301.160.70---1.84K-3416.001.701.950.732.502.80-4.28K-357.701.401.184.841.202.80-3.19CR-1-1.001.45-1.20--1.22K-371.601.200.850.821.002.40-1.31 According to Croatian legislative (water quality standards) [7], for surface waters threshold value for Hg is 1.0 gL-1 = 1000 ngL-1. In comparison with that all measured Hg values in Krka and Zrmanja river waters are extremely low, up to three orders of magnitude lower than threshold value. With respect to Hg concentrations in water, Krka River and their tributaries represent an extremely pristine environment. Mercury concentrations in sediments and tufa In Table 2 are presented mercury concentrations in sediments of Krka River, while in Table 3 are presented mercury concentrations in tufa samples. Table 2. Mercury concentrations in sediments of Krka River SampleK-04K-05 K-06K-07K-06 K-09 K-10 K-11 K-12 K-16K-17 Hg (mgkg-1)0.0140.0460.0510.0540.070.0660.0820.1340.0920.0180.027continued SampleK-18 K-19 K-20 K-21K-23 K-26 K-27 K-28 K-29 K-33 K-36 Hg (mgkg-1)0.0310.0290.0330.0190.0560.0280.0330.0840.0170.0930.048 Table 3. Mercury concentrations in tufa of Krka River SampleKR-1 KR-2 KR-3 KR-4KR-5KR-6KR-7KR-8KR-9K-02Hg (mgkg-1)0.0570.0160.0120.0140.0080.0090.0290.0180.01370.025continued SampleK-04K-12K-13K-15K-22K-25K-33K-37Hg (mgkg-1)0.0280.05640.0150.0440.0690.0080.0920.029continued SampleZR-1ZR-2ZR-3ZR-4CR-1Hg (mgkg-1)0.01350.0520.030.0910.031 Concentrations of Hg in all studied sediment and tufa samples are very low. On all locations they are far below proposed threshold value for freshwater sediments in Croatia [8]. A statistical boxplot analysis, which included all sediment and tufa data, was performed to determine if there are present some anomalies and is presented in Figure 2. All statistical analyses are performed using program Statistica 6 [9].  EMBED STATISTICA.Graph \s  Figure 2. Scatterplot with Box plots of Hg (mgkg-1) against Hg (mgkg-1) in sediments and tufa of Krka River Hg in sediments and tufa of Krka River has a positively skewed normal distribution (Skewness = 1.045). It shows only one outlier (anomaly of lower degree), which is present in sediment of K-11 location. That location is situated in most downstream part of upper Brljan Lake and receives greater part of pollution originated from city of Knin. Cluster analysis of Q-mode was also performed, and results are presented in Table 4. Table 4. Members of Clusters 1 and 2 and cluster Means (Hg mgkg-1) Cluster membersCluster MeanCluster 1k-06sed; K-07 sed; K-08 sed; K-09 sed; K-10 sed; K-11 sed; K12sed; K-23sed; K-28sed; K-22 sed; KR-1 tufa; K-26 tufa; K-22 tufa; K-24 tufa; K-23 tufa; ZR-2 tufa; ZR-1 tufa0.074612Cluster 2K-04 sed; K-05 sed; K-16 sed; K17 sed; K-18 sed; K-19 sed; K-20 sed; K-21 sed; K-26 sed; K-27 sed; K-29 sed; K-36 sed; KR-02 tufa; KR-03 tufa; KR-04 tufa; KR-05 tufa; KR-06 a tufa; KR-07 tufa; KR-08 tufa; KR-09 slap tufa; K-02 tufa; K-04 tufa; K-13 tufa; K-15 tufa; K-25 tufa; K-13 tufa; K-15tufa; K-25 tufa; K-37 tufa; ZR-1 tufa; ZR-3 tufa; CTR-1 tufa0.023537Cluster analysis of Q-mode showed that two distinctive cluster exist. Both have very low Mean Hg concentrations, although Mean of Cluster 1 is more than 3 times higher than Mean of Cluster 2. This is the sign of anthropogenic influence in Cluster 1, which contains 17 locations, while anthropogenically unaffected Cluster 2 contains 32 locations. Most of samples from Cluster 1 are located around Brljan Lake, what indicates that upstream contamination, which mostly originates from Knin town, precipitates in Brljan Lake. This acts as a self-purification mechanism, what is especially good for National Park Krka, as most contamination is not transported further downstream to most important parts of park. Also, to repeat once more, although in Cluster 1 anthropogenic influence is obvious, in total it is very low. So even the samples with highest Hg-concentrations belong to very clean sediments and are far below proposed threshold value for Croatian freshwater sediments. To demonstrate how pristine Krka River is, a comparison with rather clean Kupa River drainage basin, which is situated in middle part of Croatia and parts of neighbouring Slovenia and Bosnia and Herzegovina, will be performed. Mean Hg concentration in anthropogenically unaffected cluster of sediment samples from Kupa River drainage basin is 0.08685 mgkg-1 [10]. That is a bit higher than Mean Hg concentration in anthropogenically affected Cluster 1 of Krka River (0.074612 mgkg-1), while it is about 4 times higher than Mean Hg concentration in clean Cluster 2 of Krka River. This is mostly due to local composition of rocks, as in upper part of Kupa River drainage basin there are some Hg ore occurrences, while around Krka River there are mostly pure carbonates, which contain very low concentration of Hg. Concentrations measured in current study are similar to those reported in 2002 for estuarine part of Krka River [11]. CONCLUSION Mercury concentrations were obtained in surface sediments and were compared with those in the recent tufa and with those in river water to determine the state of pollution with respect to Hg in the Krka River within the National Park Krka. Following conclusions were obtained: In comparison with Croatian water quality standards, all measured Hg values in Krka and Zrmanja river waters are extremely low, up to three orders of magnitude lower than threshold value. With respect to Hg concentrations in water of Krka River and their tributaries represent an extremely pristine environment. Concentrations of Hg in all studied sediment and tufa samples are very low, they are far below proposed threshold value for freshwater sediments in Croatia. It was shown that Hg in sediments and tufa of Krka River has a positively skewed normal distribution. Boxplot method revealed that Hg shows only one outlier (anomaly of lower degree), which is present in sediment of K-11 location. That location is situated in most downstream part of upper Brljan Lake and receives greater part of pollution originated from city of Knin. Cluster analysis of Q-mode showed that two distinctive cluster exist. Both have very low Mean Hg concentrations, although Mean of Cluster 1 is more than 3 times higher than Mean of Cluster 2, what is the sign of anthropogenic influence in Cluster 1. Final conclusion of our research is that Krka River is extremely clean river with respect to Hg. Even the anthropogenically influenced Cluster 1 from Krka River has lower concentrations than cleanest cluster from Kupa River, with which a comparison was performed. ACKNOWLEDGEMENTS The financial support of the National Park Krka, under Project Geochemistry of EcotoxicMetals in the National Park of Krka is gratefully acknowledged. REFERENCES [1] Bonacci O., Juki D., Ljubenkov I., Definition of catchment area in karst: case of the rivers Kr i and Krka, Croatia, Hydrological Sciences Journal  Journal Des Sciences Hydrologiques, vol. 51(4), pp. 682-699, 2006. [2] Bonacci O., Ljubenkov I., Roje-Bonacci, T., Karst flash floods: an example from the Dinaric karst (Croatia), Nat. Hazards and Earth System Sci., vol. 6, pp. 195-203, 2006. [3] Lojen S., Dolenec T., Vokal B., Cukrov N., Mihel i G., Papesch W., C and O stable isotope variability in recent freshwater carbonates (River Krka, Croatia), Sedimentology, vol. 51, pp 361375, 2004. 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