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Micro-pollutants in sediment samples in the middle Danube region, Serbia: occurrence and risk assessment

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Abstract

This is the first comprehensive study on the occurrence of 940 semi-volatile organic compounds including sterols, polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), pesticides, plasticizers, and other emerging compounds in 10 river and canal sediments collected in northern Serbia. For quantification of investigated compounds GC-MS-MS (selected reaction monitoring) and GC-MS (using both selected ion monitoring and total ion monitoring) methods were used. The number of detected compounds was in the range of 85–117, while the sum of the concentrations varied from 959 μg/kg dry-wt to 84,445 μg/kg dry-wt. Sterols were quantified with high frequency in nearly 100% of investigated samples suggesting that the studied rivers and canals have been contaminated by sewage. Regarding persistent organic compounds, p,p′-DDE, p,p′-DDD, and o,p′-DDT were the dominant members of organochlorine pesticides (OCPs). The concentration range of 11 quantified pesticides of 452 analyzed was from 0.564 to 61.6 μg/kg dry-wt, while the concentration range of 47 quantified PCBs of 90 analyzed was from 0.928 to 32.1 μg/kg dry-wt. OCPs (DDE, DDD, and γ-HCH) and several PAHs (fluoranthene, pyrene, phenanthrene, chrysene, benzo(a)anthracene, benzo(a)pyrene) exceeded the maximum values of the sediment quality guidelines. Contents of domestic compounds comprise a large proportion of the total contaminant concentration. Overall, the study reveals that river sediments in Vojvodina Province were moderately polluted mainly by domestic wastewater. The toxic equivalent quantity (TEQ) relative to benzo(a)pyrene and 2,3,7,8-tetrachlorodibenzodioxin for seven carcinogenic PAHs and six quantified dioxin-like PCBs ranged from 3.59 to 103 μg TEQ/kg and from 0.001 × 10−3 to 2.10 × 10−3 μg TEQ/kg, respectively, and were in the range or lower than the literature published data.

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References

  • Acquavita A, Falomo J, Predonzani S, Tamberlich F, Bettoso N, Mattassi G (2014) The PAH level, distribution and composition in surface sediments from a Mediterranean lagoon: the Marano and Grado Lagoon (Northern Adriatic Sea, Italy). Mar Pollut Bull 81:234–241

    Article  CAS  Google Scholar 

  • Antonijević MD, Arsović M, Čáslavsky J, Cvetković V, Dabić P, Franko M, Ilić G, Ivanović M, Ivanović N, Kosovac M, Medić D, Najdanović S, Nikolić M, Novaković J, Radovanović T, Ranić Đ, Šajatović B, Špijunović G, Stankov I, Tošović J, Trebše P, Vasiljević O, Schwarzbauer J (2014) Actual contamination of the Danube and Sava Rivers at Belgrade. J Serb Chem Soc 79:1169–1184

    Article  CAS  Google Scholar 

  • Babić-Mladenović M, Kolarov V, Damjanović V (2013) Sediment regime of the Danube River in Serbia. Int J Sediment Res 28:470–485

    Article  Google Scholar 

  • Bajt O (2014) Aliphatic and polycyclic aromatic hydrocarbons in Gulf of Trieste sediments (northern Adriatic): potential impacts of maritime traffic. Bull Enviro. Contam. Toxicology 93:299–305

    CAS  Google Scholar 

  • Bergemann M, Gaumert T, Wasserguetestelle E (2008) Hamburg. http://www.fgg-elbe.de/dokumente/gewaesserguete.html

  • Cachada A, Pato P, Rocha-Santos T, Ferreira da Silva E, Duarte AC (2012) Levels, sources and potential human health risks of organic pollutants in urban soils. Sci Total Environ 430:184–192

    Article  CAS  Google Scholar 

  • Colombo JC, Pelletier E, Brochu C, Khalll M, Catoggio JA (1989) Determination of hydrocarbon sources using n-alkane and polyaromatic hydrocarbon distribution indexes. Case study: Rio La Plate estuary Argentina. Environ Sci Technol 23:888–894

    Article  CAS  Google Scholar 

  • Duong HT, Kadokami K, Chau HTC, Nguyen TQ, Nguyen TT, Kong L (2015) Groundwater screening for 940 organic micro-pollutants in Hanoiand Ho Chi Minh City, Vietnam. Environ Sci Pollut Res 22:19835–19847

    Article  CAS  Google Scholar 

  • Duong HT, Kadokami K, Pan S, Matsuura N, Nguyen TQ (2014) Screening and analysis of 940 organic micro-pollutants in river sediments in Vietnam using an automated identification and quantification database system for GC–MS. Chemosphere 107:462–472

    Article  CAS  Google Scholar 

  • EQS, Environmental Quality Standards, Substance Data Sheet. Diethylhexylphthalate (DEHP), Common implementation strategy for the water framework directive, Final version Brussels, 31 July 2005

  • Fujii Y, Haraguchi K, Harada KH, Hitomi T, Inoue K, Itoh Y, Watanabe T, Takenaka K, Uehara S, Yang HR, Kim MY, Moon CS, Kim HS, Wang P, Liu A, Hung N, Koizumi A (2011) Detection of DCF and related pesticides in human breast milk from China, Korea and Japan. Chemosphere 82:25–31

    Article  CAS  Google Scholar 

  • Furtula V, Liu J, Chambers P, Osachoff H, Kennedy C, Harkness J (2012) Sewage treatment plants efficiencies in removal of sterols and sterol ratios as indicators of fecal contamination sources. Water Air Soil Pollut 223:1017–1031

    Article  CAS  Google Scholar 

  • Hitch RK, Day HR (1992) Unusual persistence of DDT in some western USA soils. Bull Environ Contam Toxicol 48:259–264

    Article  CAS  Google Scholar 

  • Iwata H, Tanabe S, Sakai N, Tatsukawa R (1993) Distribution of persistent organochlorines in the oceanic air and surface seawater and the role of ocean on their global transport and fate. Environ Sci Technol 27:1080–1098

    Article  CAS  Google Scholar 

  • JDS1, Summary of the Final Report Joint Danube Survey (2002) ICPDR—International Commission for the Protection of the Danube River / Permanent Secretariat Vienna International Centre, D0412 P. O. Box 500, 1400 Vienna / Austria

  • JDS2, Joint Danube Survey 2, Final Scientific Report, 2008, ICPDR—International Commission for the Protection of the Danube River / Permanent Secretariat Vienna International Centre, D0412 P. O. Box 500, 1400 Vienna / Austria

  • JDS3, Joint Danube Survey 3, A Comprehensive Analysis of Danube Water Quality, 2015, ICPDR—International Commission for the Protection of the Danube River / Permanent Secretariat Vienna International Centre, D0412 P. O. Box 500, 1400 Vienna / Austria

  • Kadokami K, Tanada K, Taneda K, Nakagawa K (2005) Novel gas chromatography–mass spectrometry database for automatic identification and quantification of micropollutants. J Chromatogr A 1089:219–226

    Article  CAS  Google Scholar 

  • Kadokami K, Li X, Pan S, Ueda N, Hamada K, Jinya D, Iwamura T (2013) Screening analysis of hundreds of sediment pollutants and evaluation of their effects on benthic organisms in Dokai Bay, Japan. Chemosphere 90:721–728

    Article  CAS  Google Scholar 

  • Kadokami K, Pan S, Hanh DT, Li X, Miyazaki T (2012) Development of a comprehensive analytical method for semi-volatile organic compounds in sediments by using an automated identification and quantification system with a GC-MS database. Anal Sci 28:1183–1189

    Article  CAS  Google Scholar 

  • Kanzari F, Syakti AD, Asia L, Malleret L, Mille G, Jamoussi B, Abderrabba M, Doumenq P (2012) Aliphatic hydrocarbons, polycyclic aromatic hydrocarbons, polychlorinated biphenyls, organochlorine, and organophosphorous pesticides in surface sediments from the Arc river and the Berre lagoon, France. Environ Sci Pollut Res 19:559–576

    Article  CAS  Google Scholar 

  • Kanzari F, Asia L, Syakti D, Piram A, Malleret L, Mille G, Doumenq P (2015) Distribution and risk assessment of hydrocarbons (aliphatic and PAHs), polychlorinated biphenyls (PCBs), and pesticides in surface sediments from an agricultural river (Durance) and an industrialized urban lagoon (Berre lagoon), France. Environ Monit Assess 187:591

    Article  CAS  Google Scholar 

  • Kanzari F, Syakti AD, Asia L, Malleret L, Piram A, Mille G, Doumenq P (2014) Distributions and sources of persistent organic pollutants (aliphatic hydrocarbons, PAHs, PCBs and pesticides) in surface sediments of an industrialized urban river (Huveaune), France. Sci Total Environ 478:141–151

    Article  CAS  Google Scholar 

  • Kong K, Kadokami K, Duong HT, Chau HTC (2016) Screening of 1300 organic micro-pollutants in groundwater from Beijing and Tianjin, North China. Chemosphere 165:221–230

    Article  CAS  Google Scholar 

  • Kong L, Kadokami K, Wang S, Duong HT, Chau HTC (2015) Monitoring of 1300 organic micro-pollutants in surface waters from Tianjin, North China. Chemosphere 122:125–130

    Article  CAS  Google Scholar 

  • Kukučka P, Audy O, Kohoutek J, Holt E, Kalábová T, Holoubek I, Klánová J (2015) Source identification, spatio-temporal distribution and ecological risk of persistent organic pollutants in sediments from the upper Danube catchment. Chemosphere 138:777–783

    Article  CAS  Google Scholar 

  • Liu H, Liang H, Liang Y, Zhang D, Wang C, Cai H, Shvartsev SL (2010) Distribution of phthalate esters in alluvial sediment: a case study at JiangHan Plain, Central China. Chemosphere 78:382–388

    Article  CAS  Google Scholar 

  • Liu Y, Beckingham B, Ruegner H, Li Z, Ma L, Schwientek M, Xie H, Zhao J, Grathwohl P (2013) Comparison of sedimentary PAHs in the rivers of Ammer (Germany) and Liangtan (China): differences between early- and newly-industrialized countries. Environ Sci Technol 47:701–709

    Article  CAS  Google Scholar 

  • Long ER, Morgan LG (1991) The potential for biological effects of sediment-sorbed contaminants tested in the National Status and Trends Program. NOAA Technical Memorandum NOS OMA 52. National Oceanic and Atmospheric Administration. Seattle, Washington. US government printing office: 1990-792-615223032.

  • Loos R, Gawlik BM, Locoro G, Rimaviciute E, Contini S, Bidoglio G (2009) EU-wide survey of polar organic persistent pollutants in European river waters. Environ Pollut 157:561–568

    Article  CAS  Google Scholar 

  • MacDonald DD, Ingersoll CG, Smorong DE, Lindskoog RA, Sloane G, Biernacki T (2003) Development and evaluation of numerical sediment quality assessment guidelines for Florida Inland waters. Technical Report, Florida Department of Environmental Protection, Florida

    Google Scholar 

  • Matić-Bujagić I, Grujić S, Jauković Z, Laušević M (2016) Sterol ratios as a tool for sewage pollution assessment of river sediments in Serbia. Environ Pollut 213:76–83

    Article  CAS  Google Scholar 

  • Meffe R, de Bustamante I (2014) Emerging organic contaminants in surface water and groundwater: a first overview of the situation in Italy. Sci Total Environ 481:280–295

    Article  CAS  Google Scholar 

  • Micić V, Hofmann T (2009) Occurrence and behaviour of selected hydrophobic alkylphenolic compounds in the Danube River. Environ Pollut 157:2759–2768

    Article  CAS  Google Scholar 

  • Minissi S, Caccese D, Passafiume F, Grella A, Eleonora C, Rizzoni M (1998) Mutagenicity (micronucleus test in Vicia faba root tips), polycyclic aromatic hydrocarbons and heavy metal content of sediments collected in Tiber river and its tributaries within the urban area of Rome. Mutat Res 420:77–84

    Article  CAS  Google Scholar 

  • Montuori P, Aurino S, Garzonio F, Sarnacchiaro P, Nardone A, Triassi M (2016a) Distribution, sources and ecological risk assessment of polycyclic aromatic hydrocarbons in water and sediments from Tiber River and estuary, Italy. Sci Total Environ 566-567:1254–1267

    Article  CAS  Google Scholar 

  • Montuori P, Aurino S, Garzonio F, Triassi M (2016b) Polychlorinated biphenyls and organochlorine pesticides in Tiber River and Estuary: occurrence, distribution and ecological risk. Sci Total Environ 571:1001–1016

    Article  CAS  Google Scholar 

  • Nagy AS, Szabó J, Vass I (2014) Occurrence and distribution of polycyclic aromatic hy- drocarbons in surface water and sediments of the Danube River and its tributaries, Hungary. J Environ Sci Health A Tox Hazard Subst Environ Eng 49:1134–1141

    Article  CAS  Google Scholar 

  • Natchkov I, Case Study IX - The Danube Basin, water pollution control—a guide to the use of water quality management principles, Edited by Richard Helmer and Ivanildo Hespanhol, Published on behalf of the United Nations Environment Programme, the Water Supply & Sanitation Collaborative Council and the World Health Organization by E. & F. Spon © 1997 WHO/UNEP ISBN 0 419 22910 8

  • Oliva AL, Quintas PY, La Colla NS, Arias AH, Marcovecchio JE (2015) Distribution, sources, and potential ecotoxicological risk of polycyclic aromatic hydrocarbons in surface sediments from Bahía Blanca Estuary, Argentina. Arch Environ Contam Toxicol 69:163–172

    Article  CAS  Google Scholar 

  • Pan S, Kadokami K, Li X, Duong HT, Horiguchi T (2014) Target and screening analysis of 940 micro-pollutants in sediments in Tokyo Bay, Japan. Chemosphere 99:109–116

    Article  CAS  Google Scholar 

  • Patrolecco L, Ademollo N, Capri S, Pagnotta R, Polesello S (2010) Occurrence of priority hazardous PAHs in water, suspended particulate matter, sediment and common eels (Anguilla anguilla) in the urban stretch of the River Tiber (Italy). Chemosphere 81:1386–1392

    Article  CAS  Google Scholar 

  • Pérez F, Llorca M, Köck-Schulmeyerv M, Škrbić B, Oliveira LS, Martinello KDB, Al-Dhabi NA, Antić I, Farréa M, Barceló D (2014) Assessment of perfluoroalkyl substances in food items at global scale. Environ Res 135:181–189

    Article  CAS  Google Scholar 

  • Pérez-Fernández B, Viñas L, Franco MÁ, Bargiela J (2015) PAHs in the Ría de Arousa (NW Spain): a consideration of PAHs sources and abundance. Mar Pollut Bull 95:155–165

    Article  CAS  Google Scholar 

  • Petrović M, Škrbić B, Živančev J, Ferrando-Climent L, Barcelo D (2014) Determination of 81 pharmaceutical drugs by high performance liquid chromatography coupled to mass spectrometry with hybrid triple quadrupole–linear ion trap in different types of water in Serbia. Sci Total Environ 468–469:415–428

    Article  CAS  Google Scholar 

  • Qi W, Liu H, Qu J, Ren H, Xu W (2011) PAH desorption from sediments with different contents of organic carbon from wastewater receiving rivers. Environ Sci Pollut Res 18:346–354

    Article  CAS  Google Scholar 

  • Qiu X, Zhu T, Yao B, Hu J, Hu S (2005) Contribution of dicofol to the current DDT pollution in China. Environ Sci Technol 39:4385–4390

    Article  CAS  Google Scholar 

  • Quémenéur M, Marty Y (1994) Fatty-acids and sterols in domestic wastewaters. Water Res 28:1217–1226

    Article  Google Scholar 

  • Salo S, Verta M, Malve O, Korhonen M, Lehtoranta J, Kiviranta H, Isosaari P, Ruokojarvi P, Koistinen J, Vartiainen T (2008) Contamination of River Kymijoki sediments with polychlorinated dibenzo-p-dioxins, dibenzofurans and mercury and their transport to the Gulf of Finland in the Baltic Sea. Chemosphere 73:1675–1683

    Article  CAS  Google Scholar 

  • Sanders JM, Bucher JR, Peckham JC, Kissling GE, Hejtmancik MR, Chhabra RS (2009) Carcinogenesis studies of cresols in rats and mice. Toxicology 257:33–39

    Article  CAS  Google Scholar 

  • Sarria-Villa R, Ocampo-Duque W, Páez M, Schuhmacher M (2016) Presence of PAHs in water and sediments of the Colombian Cauca River during heavy rain episodes, and implications for risk assessment. Sci Total Environ 540:455–465

    Article  CAS  Google Scholar 

  • Schröder P, Helmreich B, Škrbić B, Carballa M, Papa M, Pastore C, Emre Z, Oehmen A, Langenhoff A, Molinos M, Dvarioniene J, Huber C, Tsagarakis KP, Martinez-Lopez E, Meric Pagano S, Vogelsang C, Mascolo G (2016) Status of hormones and painkillers in wastewater effluents across several European states—considerations for the EU watch list concerning estradiols and diclofenac. Environ Sci Pollut Res 23:12835–12866

    Article  CAS  Google Scholar 

  • Schwarzenbach RP, Escher BI, Fenner F, Hofstetter CTB, Johnson A, von Gunten U, Wehrli B (2009) The challenge of micropollutants in aquatic systems. Science 313:1072–1077

    Article  CAS  Google Scholar 

  • Škrbić B, Cvejanov J, Đurišić-Mladenović N (2007) Organochlorine pesticides and polychlorinated biphenyls in surface soils of Novi Sad and bank sediment of the Danube River. J Environ Sci Health B 42:311–319

    Article  CAS  Google Scholar 

  • Škrbić B, Cvejanov J, Đurišić-Mladenović N (2005a) Polycyclic aromatic hydrocarbons in surface soils of Novi Sad and bank sediment of the Danube River. J Environ Sci Health A 40:29–42

  • Škrbić B, Đurišić-Mladenović N (2007) Principal component analysis for soil contamination with organochlorine compounds. Chemosphere 68:2144–2152

    Article  CAS  Google Scholar 

  • Škrbić B, Đurišić-Mladenović N, Cvejanov J (2005b) Principal component analysis of trace elements in Serbian wheat. J Agr Food Chem 53:2171–2175

    Article  CAS  Google Scholar 

  • Škrbić B, Ji Y, Đurišić-Mladenović N, Zhao J (2016) Occurrence of the phthalate esters in soil and street dust samples from the Novi Sad city area, Serbia, and the influence on the children’s and adults’ exposure. J Hazard Mater 312:272–279

  • Škrbić B, Marinković V, Antić I, Petrović-Gegić A (2017) Seasonal variation and health risk assessment of organochlorine compounds in urban soils of Novi Sad, Serbia. Chemosphere 181:101–110

    Article  CAS  Google Scholar 

  • Smith SL, MacDonald DD, Keenleyside KA, Ingersoll CG, Field J (1996) A preliminary evaluation of sediment quality assessment values for freshwater ecosystems. J Great Lakes Res 22:624–638

    Article  CAS  Google Scholar 

  • Stuart M, Lapworth D, Crane E, Hart A (2012) Review of risk of from potential emerging contaminants in UK groundwater. Sci Total Environ 416:1–21

    Article  CAS  Google Scholar 

  • Syed JH, Malik RN, Li J, Chaemfa C, Zhang G, Jones KC (2014) Status, distribution and ecological risk of organochlorines (OCs) in the surface sediments from the Ravi River, Pakistan. Sci Total Environ 472:204–211

    Article  CAS  Google Scholar 

  • Takasuga T, Senthilkumar K, Matsumura T, Shiozaki K, Sakai S (2006) Isotope dilution analysis of polychlorinated biphenyls (PCBs) in transformer oil and global commercial PCB formulations by high resolution gas chromatography- high resolution mass spectrometry. Chemosphere 62:469–484

    Article  CAS  Google Scholar 

  • Torres JPM, Pfeiffer WC, Markowitz S, Pause R, Malm O, Japenga J (2002) Dichlorodiphenyltrichloroethane in soil, river sediment, and fish in the Amazon in Brazil. Environ Res 88:134–139

    Article  CAS  Google Scholar 

  • Unice KM, Kreider ML, Panko JM (2012) Use of a deuterated internal standard with pyrolysis-GC/MS dimeric marker analysis to quantify tire tread particles in the environment. Int J Environ Res Public Health 9:4033–4055

    Article  CAS  Google Scholar 

  • Unice KM, Bare JL, Kreider ML, Panko JM (2015) Experimental methodology for assessing the environmental fate of organic chemicals in polymer matrices using column leaching studies and OECD 308 water/sediment systems: application to tire and road wear particles. Sci Total Environ 533:476–487

    Article  CAS  Google Scholar 

  • Wang J, Bo L, Li L, Wang D, Chen G, Christie P, Teng Y (2014) Occurrence of phthalate esters in river sediments in areas with different land use patterns. Sci Total Environ 500–501:113–119

    Article  CAS  Google Scholar 

  • Yunker MB, Macdonald RW, Vingarzan R, Mitchell RH, Goyette D, Sylvestre S (2002) PAHs in the Fraser River basin: a critical appraisal of PAH ratios as indicators of PAH source and composition. Org Geochem 33:489–451

    Article  CAS  Google Scholar 

  • Zakaria MP, Takada H, Tsutsumi S, Ohno K, Yamada J, Kouno E, Kumata H (2002) Distribution of polycyclic aromatic hydrocarbons (PAHs) in rivers and estuaries in Malaysis: a widespread input of petrogenic PAH. Environ Sci Technol 36:1907–1918

    Article  CAS  Google Scholar 

  • Zhang Z, Huang J, Yu G, Hong H (2004) Occurrence of PAHs, PCBs and organochlorine pesticides in the Tonghui River of Beijing, China. Environ Pollut 130:249–261

    Article  CAS  Google Scholar 

Download references

Acknowledgements

Biljana Škrbić would like to thank the Japanese Society for the Promotion of Science Fellow Program 2014 for granting her fellowship to the University of Kitakyushu, Kitakyushu, Japan. The parts of this investigation were obtained within the project no. 172050 supported by the Ministry of Education, Science and Technological Development of the Republic of Serbia.

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  1. Faculty of Technology, Laboratory for Chemical Contaminants and Sustainable Development, University of Novi Sad, Bulevar cara Lazara 1, Novi Sad, 21000, Serbia

    Biljana D. Škrbić & Igor Antić

  2. Institute of Environmental Engineering, University of Kitakyushu, 1-1 Hibikino, Wakamatsu, Kitakyushu, Fukuoka, 808-0135, Japan

    Kiwao Kadokami

  3. Faculty of Medicine, University of Novi Sad, Hajduk Veljkova 3, 21000, Novi Sad, Republic of Serbia

    Grigorije Jovanović

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  1. Biljana D. Škrbić
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  2. Kiwao Kadokami
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Škrbić, B.D., Kadokami, K., Antić, I. et al. Micro-pollutants in sediment samples in the middle Danube region, Serbia: occurrence and risk assessment. Environ Sci Pollut Res 25, 260–273 (2018). https://doi.org/10.1007/s11356-017-0406-3

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