Advertisement

Environmental Science and Pollution Research

, Volume 25, Issue 34, pp 34519–34530 | Cite as

Transport of polycyclic aromatic hydrocarbons in a highly vulnerable karst underground river system of southwest China

  • Jiacheng Lan
  • Yuchuan Sun
  • Daoxian Yuan
Research Article
  • 51 Downloads

Abstract

The concentration and fluxes of polycyclic aromatic hydrocarbons (PAHs) were investigated in a karst underground river system in southwest China. Groundwater, particles, and sediments from underground river, topsoil, and surface water were monitored, allowing establishment of a conceptual model of PAH transport at the watershed scale. The results showed that PAHs could be transported from the surface to the subsurface through two migration pathways, which were slow-flowing water in the karst fissure and fast-flowing water in conduits. During rainfall events, increasing PAH levels (concentrations and fluxes) at the underground river exit indicated that hydrodynamic force could facilitate PAH transport. The PAHs in water were dominated by dissolved PAHs, accounting for 58.7% of total, especially in the freely dissolved phase, in which SPM-associated PAHs accounted for 41.3% of the total PAHs. Low molecular weight PAHs dominated transport and were mainly transported in dissolved form, whereas high molecular weight PAHs were dominated by SPM-associated transport during the rainfall events. A significantly positive correlation was observed between two-ring and three-ring freely dissolved PAHs and dissolved organic carbon (p < 0.01), respectively. Moreover, PAHs with four to five rings were relatively more abundant in the dissolved organic matter (DOM) associated phase than in the freely dissolved phase, suggesting a major role of DOM in their transport during rainfall events. The trend of PAH fluxes suggested that particle-facilitated transport was another dominant cause of PAH mobilization.

Keywords

Polycyclic aromatic hydrocarbons Particle-facilitated transport DOM-facilitated transport Conceptual model Karst underground river system Rainfall events 

Notes

Acknowledgments

The authors give thanks to State Engineering Technology Institute for Karst Desertification control, Guizhou, China and Chongqing Key Laboratory of Karst Environment, Chongqing, China. The authors also give thanks to all the schoolmasters and co-workers. The authors would like to thank LetPub (www.letpub.com) for providing linguistic assistance during the preparation of this manuscript.

Funding information

This study was financially supported by Chinese Nation Nature Fund (No. 41761091, No. 41601584), the National Key Research and Development Project of China (No. 2016YFC0502603), Guizhou Province Science and Technology Fund (No. Qiankehe Foundation [2017]1417, Qiankehe J [2015]2111), Geological Survey Project of Ministry of Land and Resources of the People’s Republic of China (DD20160305), domestic first-class discipline construction project in Guizhou (Geography of Guizhou Normal University, No. Qiankehe Research Foundation [2017] 85), and Guizhou Normal University Doctoral Research Fund (No. 2015).

References

  1. Einsiedl F, Radke M, Maloszewski P (2010) Occurrence and transport of pharmaceuticals in a karst groundwater system affected by domestic wastewater treatment plants. J Contam Hydrol 117:26–36CrossRefGoogle Scholar
  2. Fernandes MB, Sicre MA, Boireau A, Tronczynski J (1997) Polyaromatic hydrocarbon (PAH) distributions in the Seine River and its estuary. Mar Pollut Bull 34:857–867CrossRefGoogle Scholar
  3. Flynn RM, Sinreich M (2010) Characterisation of virus transport and attenuation in epikarst using short pulse and prolonged injection multi-tracer testing. Water Res 44:1138–1149CrossRefGoogle Scholar
  4. Ford DC, Williams P (2007) Karst hydrogeology and geomorphology. Wiley & Sons, ChichesterCrossRefGoogle Scholar
  5. Goldscheider N, Meiman J, Pronk M, Smart C (2008) Tracer tests in karst hydrogeology and speleology. Int J Speleol 37:27–40CrossRefGoogle Scholar
  6. Johnsen AR, Karlson U (2007) Diffuse PAH contamination of surface soils: environmental occurrence, bioavailability, and microbial degradation. Appl Microbiol Biotechnol 76:533–543CrossRefGoogle Scholar
  7. Kogovsek J, Petric M (2014) Solute transport processes in a karst vadose zone characterized by long-term tracer tests (the cave system of Postojnska Jama, Slovenia). J Hydrol 519:1205–1213CrossRefGoogle Scholar
  8. Kong X, Qi S, Oramah IT, Zhang Y, He S (2011) Contamination of polycyclic aromatic hydrocarbons in surface water in underground river of Dashiwei Tiankeng group in karst area, Guangxi. Environ Sci 32:1081–1087 (in Chinese with English abstract)Google Scholar
  9. Kong X, Qi S, Jiang Z, Huang B (2012) Environmental factors on distribution of polycyclic aromatic hydrocarbons in soils from Dashiwei karst giant doline (Tiankeng) in Guangxi, China. Environ Sci 33:3905–3915 in Chinese with English abstractGoogle Scholar
  10. Lan J, Sun Y, Tian P, Lu B, Shi Y, Xu X, Liang Z, Yang P (2014) Contamination and ecological risk assessment of polycylic aromatic hydrocarbons in water and in karst underground river catchment. Environ Sci 35:84–92 in Chinese with English abstractGoogle Scholar
  11. Lan J, Sun Y, Shi Y, Liang Z (2015) Contamination and ecological risk assessment of polycyclic aromatic hydrocarbons in surface sediment in karst underground river. Environ Sci 36:855–861 in Chinese with English abstractGoogle Scholar
  12. Lan J, Sun Y, Xiao S, Yuan D (2016) Polycyclic aromatic hydrocarbon contamination in a highly vulnerable underground river system in Chongqing, Southwest China. J Geochem Explor 168:65–71CrossRefGoogle Scholar
  13. Li N, Lee HK (2000) Tandem-cartridge solid-phase extraction followed by GC/MS analysis for measuring partition coefficients of association of polycyclic aromatic hydrocarbons to humic acid. Anal Chem 72:5272–5279CrossRefGoogle Scholar
  14. Ligaray M, Baek SS, Kwon H-O, Choi S-D, Cho KH (2016) Watershed-scale modeling on the fate and transport of polycyclic aromatic hydrocarbons (PAHs). J Hazard Mater 320:442–457CrossRefGoogle Scholar
  15. Maioli OLG, Rodrigues KC, Knoppers BA, Azevedo DA (2011) Distribution and sources of aliphatic and polycyclic aromatic hydrocarbons in suspended particulate matter in water from two Brazilian estuarine systems. Cont Shelf Res 31:1116–1127CrossRefGoogle Scholar
  16. Mitra S, Dickhut RM (1999) Three-phase modeling of polycyclic aromatic hydrocarbon association with pore-water-dissolved organic carbon. Environ Toxicol Chem 18:1144–1148CrossRefGoogle Scholar
  17. Moeckel C, Monteith DT, Llewellyn NR, Henrys PA, Pereira MG (2014) Relationship between the concentrations of dissolved organic matter and polycyclic aromatic hydrocarbons in a typical U.K. upland stream. Environ Sci Technol 48:130–138CrossRefGoogle Scholar
  18. Morales T, Uriarte JA, Olazar M, Antigüedad I, Angulo B (2010) Solute transport modelling in karst conduits with slow zones during different hydrologic conditions. J Hydrol 390:182–189CrossRefGoogle Scholar
  19. Morales T, Angulo B, Uriarte JA, Olazar M, Arandes JM, Antiguedad I (2017) Solute transport characterization in karst aquifers by tracer injection tests for a sustainable water resource management. J Hydrol 547:269–279CrossRefGoogle Scholar
  20. Motelay-Massei A, Garban B, Tiphagne-larcher K, Chevreuil M, Ollivon D (2006) Mass balance for polycyclic aromatic hydrocarbons in the urban watershed of Le Havre (France): transport and fate of PAHs from the atmosphere to the outlet. Water Res 40:1995–2006CrossRefGoogle Scholar
  21. Mouhri A, Motelay-massei A, Massei N, Fournier M, Laignel B (2008) Polycyclic aromatic hydrocarbon transport processes on the scale of a flood event in the rural watershed of Le Bebec, France. Chemosphere 73:443–450CrossRefGoogle Scholar
  22. Perrette Y, Poulenard J, Durand A, Quiers M, Malet E, Fanget B, Naffrechoux E (2013) Atmospheric sources and soil filtering of PAH content in karst seepage waters. Org Geochem 65:37–45CrossRefGoogle Scholar
  23. Poerschmann J, Zhang Z, Kopinke F-D, Pawliszyn J (1997) Solid phase microextraction for determining the distribution of chemicals in aqueous matrices. Anal Chem 69:597–600CrossRefGoogle Scholar
  24. Schwarz K, Gocht T, Grathwohl P (2011) Transport of polycyclic aromatic hydrocarbons in highly vulnerable karst systems. Environ Pollut 159:133–139CrossRefGoogle Scholar
  25. Shao Y, Wang Y, Xu X, Wu X, Jiang Z, He S, Qian K (2014) Occurrence and source apportionment of PAHs in highly vulnerable karst system. Sci Total Environ 490:153–160CrossRefGoogle Scholar
  26. Shevenell L, McCarthy JF (2002) Effects of precipitation events on colloids in a karst aquifer. J Hydrol 255:50–68CrossRefGoogle Scholar
  27. Shi Z, Tao S, Pan B, Liu WX, Shen WR (2007) Partitioning and source diagnostics of polycyclic aromatic hydrocarbons in rivers in Tianjin, China. Environ Pollut 146:492–500CrossRefGoogle Scholar
  28. Sun Y, Shen L, Yuan D (2013) Distributing features and source analysis of polycyclic aromatic hydrocarbons in epikarst soils. Carsologica Sinica 32:79–87 in Chinese with English abstractGoogle Scholar
  29. Sun Y, Shen L, Yuan D (2014) Contamination and source of polycyclic aromatic hydrocarbons in epikarst spring water. Environ Sci 35:2091–2098 in Chinese with English abstractGoogle Scholar
  30. Tremblay L, Kohl SD, Rice JA, Gagné J-P (2005) Effects of temperature, salinity, and dissolved humic substances on the sorption of polycyclic aromatic hydrocarbons to estuarine particles. Mar Chem 96:21–34CrossRefGoogle Scholar
  31. USEPA (1993): Provisional Guidance for Quantitative Risk Assessment of Polycyclic Aromatic Hydrocarbons. EPA/600/R-93/089. U.S. Environmental Protection Agency. Office of Research and Development,Washington, DCGoogle Scholar
  32. Wang Y, Qi S, Chen J, Oramah TI, Yuan D (2009) Concentration, distribution and sources of polyaromatic hydrocarbons in soils from the karst tiankengs, South China. Bull Environ Contam Toxicol 83:720–726CrossRefGoogle Scholar
  33. Wang Y, Xue R, Li J, Zhu H, Xu Y, Xue B, Qi S, Yuan D, Theodore OI (2011) Compositional fractionation of polyaromatic hydrocarbons in the karst soils, South China. Environ Earth Sci 66:2013–2019CrossRefGoogle Scholar
  34. Yang D, Qi SH, Zhang Y, Xing XL, Liu HX, Qu CK, Liu J, Li F (2013) Levels, sources and potential risks of polycyclic aromatic hydrocarbons (PAHs) in multimedia environment along the Jinjiang River mainstream to Quanzhou Bay, China. Mar Pollut Bull 76:298–306CrossRefGoogle Scholar
  35. Yuan D, Zhu D, Weng J (eds) (1994) Karst in China. Geological Publishing House, Peking, pp 127–164 in ChineseGoogle Scholar
  36. 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 33:489–515CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.School of Karst Science/State Engineering Technology Institute for Karst Desertification ControlGuizhou Normal UniversityGuiyangChina
  2. 2.Chongqing Key Laboratory of Karst Environment, School of Geographical ScienceSouthwest UniversityChongqingChina
  3. 3.Institute of Karst Environment and Rock Desertification RehabilitationChongqingChina
  4. 4.Institute of Karst Geology, CAGS, Karst Dynamics LaboratoryMLRGuilinChina

Personalised recommendations