Environmental Science and Pollution Research

, Volume 25, Issue 16, pp 15862–15872 | Cite as

Occurrence and toxicological assessment of polycyclic aromatic hydrocarbons (PAHs) in marine sediments under mussel farming influence

  • Begoña Pérez-Fernández
  • Lucía Viñas
  • Jesica Bargiela
Research Article


The use of marine resources for mussel culture has become increasingly important, particularly on the European Atlantic coast and notably in the Galician Rías in the northwest of Spain. Despite its importance, there is a lack of research and analysis in this area and of the potential problems that it could cause to the environment. This paper details the findings of a study that aimed to find the probable environmental impact of mussel culture activities and to evaluate the polycyclic aromatic hydrocarbon (PAH) content derived from this activity. The Ría de Arousa, where you can find over 70% of all installed rafts in Galicia, was selected for the present study, and nearly 40 marine sediment samples were collected there. The sediments were extracted by ASE (accelerated solvent extraction) procedure, and the quantification of PAHs was performed using gas chromatography coupled to mass spectrometry (GC-MS), with the aid of deuterated PAH internal standards. The total concentration of parental PAHs ranged from 11.66 to 30,272-ng g−1 dry weight (d.w.), with a mean value of 3907-ng g−1 d.w.; the concentration of alkyl PAHs varied from 3.72 to 1187-ng g−1 d.w., with a mean value of 205.1-ng g−1 d.w. Compositional patterns, principal component analysis (PCA) and hieratical cluster association (HCA) yielded a sediment classification where the mussel raft impact is pointed out. PAH ratios indicated a predominance of combustion sources, except in two samples, located in small harbors. Only one station showed total potential carcinogenic PAH values in the range that would frequently cause negative biological effects, and the toxic equivalent concentrations based on BaP equivalents identified another ten positions where biological effects would occur occasionally.


PAH Marine sediments Mussel farming Toxicology 



The authors thank M. López Rodriguez and G. Fernández Carrera and the technical staff of the Marine Pollution Department at IEO-Vigo, as well as the officers and crew of R/V José María Navaz for assistance in sample collection and preparation. Special thanks to M.A. Franco, head of the cruise in which the samples were collected and who gave us her support and help. We would also like to thank Valentín Trujillo for his collaboration in the statistical analysis of the data.

Funding information

The study was funded by a Fund Management Agreement between the IEO and the Spanish Ministry of Agriculture, Food and Environment (2010–2012).

Supplementary material

11356_2018_1737_MOESM1_ESM.docx (427 kb)
ESM 1 (DOCX 427 kb)


  1. 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 81:234–241CrossRefGoogle Scholar
  2. Ahad JME, Jautzy JJ, Cumming BF, Das B, Laird KR, Sanei H (2015) Sources of polycyclic aromatic hydrocarbons (PAHs) to northwestern Saskatchewan lakes east of the Athabasca oil sands. Org Geochem 80:35–45. CrossRefGoogle Scholar
  3. Álvarez-Salgado X a, Gago J, Mı́guez BM, Gilcoto M, Pérez FF (2000) Surface waters of the NW Iberian margin: upwelling on the shelf versus outwelling of upwelled waters from the Rı́as Baixas. Estuar Coast Shelf Sci 51(6):821–837. CrossRefGoogle Scholar
  4. Andersson JT, Achten C (2015) Time to say goodbye to the 16 EPA PAHs? Toward an up-to-date use of PACs for environmental purposes. Polycycl Aromat Compd 35(2–4):330–354. CrossRefGoogle Scholar
  5. Besada V, Sericano JL, Schultze F (2014) An assessment of two decades of trace metals monitoring in wild mussels from the Northwest Atlantic and Cantabrian coastal areas of Spain, 1991–2011. Environ Int 71C:1–12. CrossRefGoogle Scholar
  6. Boitsov S, Petrova V, Jensenc HKB, Kursheva A, Litvinenkob I, Klungsøyra J (2013) Sources of polycyclic aromatic hydrocarbons in marine sediments from southern and northern areas of the Norwegian continental shelf. Mar Environ Res 87-88:73–84CrossRefGoogle Scholar
  7. Chen C-F, Chen C-W, Dong C-D, Kao C-M (2013) Assessment of toxicity of polycyclic aromatic hydrocarbons in sediments of Kaohsiung Harbor, Taiwan. Sci Total Environ 463-464:1174–1181. CrossRefGoogle Scholar
  8. Chen C-W, Chen C-F (2011) Distribution, origin, and potential toxicological significance of polycyclic aromatic hydrocarbons (PAHs) in sediments of Kaohsiung Harbor, Taiwan. Mar Pollut Bull 63(5–12):417–423 Retrieved from CrossRefGoogle Scholar
  9. Crawford CM, Macleod CK, Mitchell IM (2003) Effects of shellfish farming on the benthic environment. Aquaculture 224(1–4):117–140. CrossRefGoogle Scholar
  10. Franco MA, Vinas L, Soriano JA, de Armas D, Gonzalez JJ, Beiras R et al (2006) Spatial distribution and ecotoxicity of petroleum hydrocarbons in sediments from the Galicia continental shelf (NW Spain) after the prestige oil spill. Mar Pollut Bull 53(5–7):260–271. CrossRefGoogle Scholar
  11. Grimalt JO, Cantón L, Alonso B (1992) Spatial and temporal variance of hydrocarbon pollution data in a coastal river-influenced sedimentary system. Environ Sci Technol 26:2240–2251CrossRefGoogle Scholar
  12. He X, Pang Y, Song X, Chen B, Feng Z, Ma Y, (2014) Distribution, sources and ecological risk assessment of PAHs in surface sediments from Guan River Estuary, China. Marine Pollution Bulletin 80:52–58.Google Scholar
  13. Iribarrren Lorenzo, D. (2010). Life cycle assessment of mussel and turbot aquacultureGoogle Scholar
  14. Liu Y, Chen L, Jianfu Z, Qinghui H, Zhiliang Z, Hongwen G (2008) Distribution and sources of polycyclic aromatic hydrocarbons in surface sediments of rivers and an estuary in Shanghai, China. Environ Pollut (Barking, Essex: 1987) 154(2):298–305. CrossRefGoogle Scholar
  15. Long ER, MacDonald DD, Smith SL, Calder FD (1995) Incidence of adverse biological effects within ranges of chemical concentrations in marine and estuarine sediments. Environ Manag 19(1):81–97CrossRefGoogle Scholar
  16. 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(2):163–172. CrossRefGoogle Scholar
  17. OSPAR. (2010). OSPAR Coordinated Environmental Monitoring Programme (CEMP). Agreement 2010-1. OSPAR CommissionGoogle Scholar
  18. Otero XL, Calvo de Anta RM, Macı́as F (2006) Sulphur partitioning in sediments and biodeposits below mussel rafts in the Rı́a de Arousa (Galicia, NW Spain). Mar Environ Res 61(3):305–325. CrossRefGoogle Scholar
  19. Otto, L. (1975). Oceanography of the Ría de Arousa (N.W. Spain)Google Scholar
  20. Pérez-Fernández B, Viñas L, Franco MA, Bargiela J (2015) PAHs in the Ría de Arousa (NW Spain): a consideration of PAHs sources and abundance. Mar Pollut Bull 95:155–165CrossRefGoogle Scholar
  21. Peters CA, Knightes CD, Brown DG (1999) Long-term composition dynamics of PAH-containing NAPLs and implications for risk assessment. Environ Sci Technol 33(24):4499–4507CrossRefGoogle Scholar
  22. Prego R, Otxotorena U, Cobelo-García A (2006) Presencia de Cr, Cu, Fe y Pb en el sedimento bajo las bateas de cultivo de mejillón (Rías de Arosa y Vigo, NO de España): ¿Es un área contaminada por metales? Presence of Cr, Cu, Fe and Pb in sediments underlying mussel-culture rafts (Arosa and Vigo rias). Ciencias Marinas 32(2B):339–349CrossRefGoogle Scholar
  23. Prieto A, Zuloaga O, Usobiaga A, Bartolomé L, Fernández LA, Etxebarria N, Ciprain E, Alonso A (2008) Levels and spatial distribution of inorganic and organic contaminants in sediments along the Bilbao estuary. Mar Pollut Bull 56(12):2094–2099 Retrieved from CrossRefGoogle Scholar
  24. Qiao M, Wang C, Huang S, Wang D, Wang Z (2006) Composition, sources, and potential toxicological significance of PAHs in the surface sediments of the Meiliang Bay, Taihu Lake, China. Environ Int 32:28–33CrossRefGoogle Scholar
  25. Rosenthal, H., Weston, D., Gowen, R., & Black, E. (1987). Environmental impact of mariculture. International Council for the Exploration of the SeaGoogle Scholar
  26. Rosón G, Alvarez-Salgado X a, Pérez FF (1997) A non-stationary box model to determine residual fluxes in a partially mixed estuary, based on both thermohaline properties: application to the Ria de Arousa (NW Spain). Estuar Coast Shelf Sci 44(3):249–262. CrossRefGoogle Scholar
  27. Rosón G, Pérez FF, Álvarez Salgado XA, Ríos AF (1991) Flujos de los aportes de agua continental a la Ría de Arousa. Scentia Marina 55(4):583–589Google Scholar
  28. Ruiz Y, Suárez P, Alonso A, Longo E, San Juan F (2014) Chemicals used for maintenance of wood rafts in mussel farms: evaluation of their potential toxic risk to mussel culture. Aquac Environ Interact 6(1):55–66. CrossRefGoogle Scholar
  29. Rullkotter J (2006) Organic matter: the driving force for early diagenesis. In: Schulz HD, Zabel M (eds) Marine geochemistry, vol 2, 2nd editio edn. Springer, Berlin Heidelberg, pp 125–168CrossRefGoogle Scholar
  30. Sitoy HS, Young AL, Tabbu MY (1983) Raft culture of mussels. Aquaculture Department, Southeast Asian Fisheries Development Center, Tigbauan, Iloilo, PhilippinesGoogle Scholar
  31. Sprovieri M, Feo ML, Prevedello L, Manta DS, Sammartino I, Tamburrino S, Marsella E (2007) Heavy metals, polycyclic aromatic hydrocarbons and polychlorinated biphenyls in surface sediments of the Naples harbour (southern Italy). Chemosphere 67:998–1009CrossRefGoogle Scholar
  32. Sun J-L, Ni H-G, Zeng H (2012) Ecological risk assessment of parent and halogenated polycyclic aromatic hydrocarbons in surface sediments from an urban river in south China. Environ Toxicol Chem / SETAC 31(8):1867–1873. CrossRefGoogle Scholar
  33. Tobiszewski M, Namiesnik J (2012) Review-PAH diagnostic ratios for the identification of pollution emission sources. Environ Pollut 162:110–119CrossRefGoogle Scholar
  34. US EPA. (1993). Provisional guidance for quantitative risk assessment of polycyclic aromatic hydrocarbonsGoogle Scholar
  35. Viguri J, Verde J, Irabien A (2002) Environmental assessment of polycyclic aromatic hydrocarbons (PAHs) in surface sediments of the Santander Bay, northern Spain. Chemosphere 48(2):157–165 Retrieved from CrossRefGoogle Scholar
  36. Vilas F, Bernabeu AM, Méndez G (2005) Sediment distribution pattern in the Rias Baixas (NW Spain): main facies and hydrodynamic dependence. J Mar Syst 54(1–4):261–276. CrossRefGoogle Scholar
  37. Viñas L, Franco MA, Gonzalez JJ (2009) Polycyclic aromatic hydrocarbon composition of sediments in the Ria de Vigo (NW Spain). Arch Environ Contam Toxicol 57(1):42–49. CrossRefGoogle Scholar
  38. Viñas L, Franco MA, Soriano JA, González JJ, Pon J, Albaigés J (2010) Sources and distribution of polycyclic aromatic hydrocarbons in sediments from the Spanish northern continental shelf. Assessment of spatial and temporal trends. Environ Pollut 158:1551–1560 Retrieved from CrossRefGoogle Scholar
  39. Wang H-S, Liang P, Kang Y, Shao D-D, Zheng GJ, Wu S-C et al (2010) Enrichment of polycyclic aromatic hydrocarbons (PAHs) in mariculture sediments of Hong Kong. Environ Pollut (Barking, Essex : 1987) 158(10):3298–3308. CrossRefGoogle Scholar
  40. Yang Z, Yang C, Wang Z, Hollebone B, Landriault M, Brown CE (2011) Oil fingerprinting analysis using commercial solid phase extraction (SPE) cartridge and gas chromatography-mass spectrometry (GC-MS). Anal Methods 3(3):628. CrossRefGoogle Scholar
  41. 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. Organic Geochemistry 33(4):489–515 Retrieved from <Go to ISI>://000175196500009CrossRefGoogle Scholar

Copyright information

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

Authors and Affiliations

  1. 1.Instituto Español de OceanografiaCentro Oceanogáfico de VigoVigoSpain

Personalised recommendations