Skip to main content

Advertisement

Log in

Occurrence and fate of selected surfactants in seawater at the outfall of the Marseille urban sewerage system

  • Original Paper
  • Published:
International Journal of Environmental Science and Technology Aims and scope Submit manuscript

Abstract

This paper describes an investigation of linear alkylbenzene sulfonates (LAS) and nonylphenol ethoxylates (NPEO) and their metabolites in the vicinity of the Marseille sewage outfall (wastewater treatment plant with a capacity of 1.860 million inhabitant equivalents, Northwestern Mediterranean, southeast of France). This analytical survey describes their occurrence in the subsurface and sea surface layers and investigates their possible fates in this marine environment. The results indicated the presence of LAS in both layers and up to 3 km from the discharge point, whereas the concentration of sulfophenyl carboxylic acids, which are the main metabolites of LAS, was only significant near the sewer outfall and in the surface layer. The NPEO were present only in minor quantities, especially near the discharge point, and no other selected metabolites were detected. The fate of the surfactants in question was then assessed by two types of experiments according to their potential means of degradation under natural conditions. Biodegradation assays were conducted according to a protocol defined by the United States Environmental Protection Agency (“Biodegradability in sea water, 835.3160”), with variations in the substrate input frequencies. Photodegradation experiments were carried out in a solar simulator reactor. These results demonstrated the low photodegradability and rapid primary biodegradation of LAS (with half-life times between 10.3 and 11.5 days) in the coastal area under study, although some LAS metabolites were more recalcitrant to biodegradation in this specific environment, which was also validated by linear alkylbenzene analysis in the two selected sediment stations.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  • Andreu V, Pico Y (2004) Determination of linear alkylbenzenesulfonates and their degradation products in soils by liquid chromatography-electrospray-ion trap multiple-stage mass spectrometry. Anal Chem 76:2878–2885

    Article  CAS  Google Scholar 

  • Bayona JM, Albaiges J, Solanas AM, Grifoll M (1986) Selective aerobic degradation of linear alkylbenzenes by pure microbial cultures. Chemosphere 15(5):595–598

    Article  CAS  Google Scholar 

  • Bellan G, Bourcier M, Salen-Picard C, Arnoux A, Casserley S (1999) Benthic ecosystem changes associated with wastewater treatment at marseille: implications for the protection and restoration of the Mediterranean coastal shelf ecosystems. Water Environ Res 71:483–493

    Article  CAS  Google Scholar 

  • Bester K, Theobald N, Schröder HF (2001) Nonylphenols, nonylphenol-ethoxylates, linear alkylbenzenesulfonates (LAS) and bis(4-chlorophenyl)-sulfone in the German Bight of the North Sea. Chemosphere 45(6–7):817–826

    Article  CAS  Google Scholar 

  • Boudenne JL, Coulomb B, Djellal L, Théraulaz F (2001) Determination of LAS in wastewater treatment plants: comparative study between conventional biodegradation testing and an alternative photo-oxidation method. Int J Environ Anal Chem 81(1):55–72

    Article  CAS  Google Scholar 

  • Castillo M, Riu J, Ventura F, Boleda R, Scheding R, Schröder HF, Nistor C, Emneus J, Eichhorn P, Knepper TP, Jonkers CCA, De Voogt P, Gonzalez-Mazo E, Leon VM, Barcelo D (2000) Inter-laboratory comparison of liquid chromatographic techniques and enzyme-linked immunosorbent assay for the determination of surfactants in wastewaters. J Chromatogr A 889:195–199

    Article  CAS  Google Scholar 

  • Di Corcia A, Samperi R, Marcomini A (1994) Aromatic surfactants and biodegradation intermediates in sewage by solid-phase extraction and LC. Environ Sci Technol 28:850–858

    Article  Google Scholar 

  • Diaz A, Ventura F, Galceran MT (2002) Simultaneous determination of estrogenic short ethoxy chain nonylphenols and their acidic metabolites in water by an in-sample derivatization/solid phase microextraction method. Anal Chem 74:3869–3876

    Article  CAS  Google Scholar 

  • Ding WH, Tzing SH (1998) Analysis of nonylphenol polyethoxylates and their degradation products in river water and sewage effluent by gas chromatography-ion trap (tandem) mass spectrometry with electron impact and chemical ionization. J Chromatogr A 824:79–86

    Article  CAS  Google Scholar 

  • Eganhouse RP, Sherblom PM (2001) Anthropogenic organic contaminants in the effluent of a combined sewer overflow: impact on Boston Harbor. Mar Environ Res 51(1):51–74

    Article  CAS  Google Scholar 

  • European Committee of Surfactants and their Organic Intermediates (CESIO), Statistics, 2008 (http://www.cefic.be/files/publications/cesio)

  • Fernandez J, Riu J, Garcia-Calvo E, Rodriguez A, Fernandez-Alba AR, Barcelo B (2004) Determination of photodegradation and ozonation by products of linear alkylbenzene sulfonates by liquid chromatography and ion chromatography under controlled laboratory experiments. Talanta 64(1):69–79

    Article  CAS  Google Scholar 

  • Gledhill W, Saeger VW, Treh ML (1991) An aquatic environmental safety assessment of linear alkylbenzene. Environ Toxicol Chem 10(2):169–178

    Article  CAS  Google Scholar 

  • Gonzalez S, Petrovic M, Barcelo D (2004) Simultaneous extraction and fate of linear alkylbenzene sulfonates, coconut diethanol amides, nonylphenol ethoxylates and their degradation products in wastewater treatment plants, receiving coastal waters and sediments in the Catalonian area (NE Spain). J Chromatogr A 1052(1–2):111–120

    Article  CAS  Google Scholar 

  • Gonzalez-Mazo E, Honing M, Barcelo D, Gomez-Parra A (1997) Monitoring long-chain intermediate products item the degradation of linear alkylbenzene sulfonates in the marine environment by solid-phase extraction followed by liquid chromatography/ionspray mass spectrometry. Environ Sci Technol 31:504–510

    Article  CAS  Google Scholar 

  • Gustafsson O, Long CM, Macfarlane J, Gschwend PM (2001) Fate of Linear alkylbenzenes released to the coastal environment near Boston Harbor. Environ Sci Technol 35(10):2040–2048

    Article  CAS  Google Scholar 

  • Hampel M, Mreno-Garrido I, Sobrino C, Lubian LM, Blasco J (2001) Acute toxicity of LAS homologues in marine microalgae: esterase activity and inhibition growth as endpoints of toxicity. Ecotox Environ Saf 48(3):287–292

    Article  CAS  Google Scholar 

  • Houde F, DeBlois C, Berryman D (2002) Liquid chromatographic-tandem mass spectrometric determination of nonylphenol polyethoxylates and nonylphenol carboxylic acids in surface waters. J Chrom A 961:245–256

    Article  CAS  Google Scholar 

  • Jahnke A, Gandrass J, Ruck W (2004) Simultaneous determination of alkylphenol ethoxylates and their biotransformation products by liquid chromatography/electrospray ionisation tandem mass spectrometry. J Chrom A 1035:115–122

    Article  CAS  Google Scholar 

  • Jobling S, Sheahan D, Osborne JA, Matthiessen P, Sumpter JP (1996) Inhibition of testicular growth in rainbow trout (Oncorhynchus mykiss) exposed to estrogenic alkylphenolic chemicals. Environ Toxicol Chem 15:194–202

    Article  CAS  Google Scholar 

  • Jonkers N, Laane R, de Voogt P (2005) Sources and fate of nonylphenol ethoxylates and their metabolites in the Dutch coastal zone of the North Sea. Mar Chem 96(1–2):115–135

    Article  CAS  Google Scholar 

  • Koh YK, Chiu TY, Boobis AR, Cartmell E, Pollard SJT, Scrimshaw MD, Lester JN (2008) A sensitive and robust method for the determination of alkylphenol polyethoxylates and their carboxylic acids and their transformation in a trickling filter wastewater treatment plant. Chemosphere 73:551–556

    Article  CAS  Google Scholar 

  • Lara-Martin PA, Gomez-Parra A, Gonzalez-Mazo E (2008a) Reactivity and fate of synthetic surfactants in aquatic environments. Trends Anal Chem 27(8):684–695

    Article  CAS  Google Scholar 

  • Lara-Martin PA, Gomez-Parra A, Gonzalez-Mazo E (2008b) Sources, transport and reactivity of anionic and non-ionic surfactants in several aquatic ecosystems in SW Spain: a comparative study. Environ Pollut 156(1):36–45

    Article  CAS  Google Scholar 

  • Lara-Martin PA, Gomez-Parra A, Sanz JL, Gonzalez-Mazo E (2010) Anaerobic degradation pathway of linear alkylbenzene sulfonates (LAS) in sulfate-reducing marine sediments. Environ Sci Technol 44:1670–1676

    Article  CAS  Google Scholar 

  • Leon SM, Gonzalez-Mazo E, Gomez-Parra A (2000) Extraction and isolation of linear alkylbenzene sulfonates and their intermediate metabolites from various marine organisms. J Chromatogr A 889(1–2):99–104

    Google Scholar 

  • Leon SM, Gomez-Parra A, Gonzalez-Mazo E (2004) Biodegradation of linear alkylbenzene sulfonates and their degradation intermediates in seawater. Environ Sci Technol 38(8):2359–2367

    Article  CAS  Google Scholar 

  • Marcomini A, Capri S, Giger W (1987) Determination of linear alkylbenzenesulphonates, alkylphenol polyethoxylates and nonylphenol in waste water by high-performance liquid chromatography after enrichment on octadecylsilica. J Chromatogr A 403:243–252

    Article  CAS  Google Scholar 

  • Marcomini A, Di Corcia A, Samperi R, Capri S (1993) Reversed-phase high-performance liquid chromatographic determination of linear alkylbenzene sulphonates, nonylphenol polyethoxylates and their carboxylic biotransformation products. J Chromatogr A 644:59–61

    Article  CAS  Google Scholar 

  • Mungray AK, Kumar P (2009) Fate of linear alkylbenzene sulfonates in the environment: a review. Int Biodeter Biodegrad 63:981–987

    Article  CAS  Google Scholar 

  • Munoz I, Gomez-Ramos MJ, Aguera A, Fernandez-Alba AR, Garcia-Reyes JF, Molina-Diaz A (2009) Chemical evaluation of contaminants in wastewater effluents and the environmental risk of reusing effluents in agriculture Trends. Anal Chem 28(6):676–694

    CAS  Google Scholar 

  • Nunez L, Turiel E, Tadeo JL (2007) Determination of nonylphenol and nonylphenol ethoxylates in environmental solid samples by ultrasonic-assisted extraction and high performance liquid chromatography-fluorescence detection. J Chromatogr A 1146:157–163

    Article  CAS  Google Scholar 

  • Perales JA, Manzano MA, Sales D, Quiroga JM (2003) Biodisposition of linear alkylbenzene sulphonates and their associated sulphophenyl carboxylic acid metabolites in sea water. Int Biodeter Biodegr 51:187–194

    Article  CAS  Google Scholar 

  • Petrovic M, Diaz A, Ventura F, Barcelo D (2001) Simultaneous determination of halogenated derivatives of alkylphenol ethoxylates and their metabolites in sludges, river sediments and surface, drinking, and wastewaters by liquid chromatography-mass spectrometry. Anal Chem 73:5886–5895

    Article  CAS  Google Scholar 

  • Prats D, Lopez C, Vallejo D, Varo P, Leon VM (2006) Effect of temperature on the biodegradation of linear alkylbenzene sulfonate and alcohol ethoxylate. J Surf Deterg 9(1):69–75

    Article  CAS  Google Scholar 

  • Sarrazin L, Arnoux A, Rebouillon P (1997) High-performance liquid chromatographic analysis of a linear alkylbenzenesulfonate an dits environmental biodegradation metabolites. J Chromatogr A 760:285–291

    Article  CAS  Google Scholar 

  • Suri M, Huld TA, Dunlop ED, Ossenbrink HA (2007) Potential of solar electricity generation in the European Union member states and candidate countries. Sol Energy 81:1295–1305

    Article  Google Scholar 

  • Swisher RD (1987) Surfactant biodegradation. Marcel Dekker, New York

    Google Scholar 

  • Takada H, Ogura N (1992) Removal of linear alkylbenzenesulfonates (LAS) in the Tamagawa estuary. Mar Chem 37:257–263

    Article  CAS  Google Scholar 

  • Tan X, Yim SY, Uppu P, Kleinow KM (2010) Enhanced bioaccumulation of dietary contaminants in catfish with exposure to the waterborne surfactant linear alkylbenzene sulfonate. Aquat Toxicol 99(2):300–308

    Article  CAS  Google Scholar 

  • Trehy ML, Gledhill WE, Orth RG (1990) Determination of linear alkylbenzenesulfonates and dialkyltetralinsulfonates in water and sediment by gas chromatography/mass spectrometry. Anal Chem 62:2581–2589

    Article  CAS  Google Scholar 

  • Tubau I, Vasquez-Sune E, Carrera J, Gonzalez S, Petrovic M, Lopez de Alda MJ, Barcelo D (2010) Occurrence and fate of alkylphenol polyethoxylate degradation products and linear alkylbenzene sulfonate surfactants in urban ground water: Barcelona case study. J Hydrol 383(1–2):102–110

    Article  CAS  Google Scholar 

  • US.EPA (1998) Fate, transport and transformation test guidelines. OPPTS 835. 3160: biodegradability in sea water. Washington, DC. http://fedbbs.access.gpo.gov/library/epa_835/835-3160.pdf, Jan 2013

  • Zgola-Grzeskowiak A, Grzeskowiak T, Rydlichowski R, Lukaszewski Z (2009) Determination of nonylphenol and short-chained nonylphenol ethoxylates in drain water from an agricultural area. Chemosphere 75:513–518

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This research was supported by a grant from the Rhone-Mediterranean and Corsica Water Agency (Grant 2009-1316). This work was partially supported by ANR project MARSECO (ANR-CESA-018-06). We acknowledge Ms. Valentini-Poirier and Mr. Boissery for sparking our interest in this study.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to J.-L. Boudenne.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Robert-Peillard, F., Syakti, A.D., Coulomb, B. et al. Occurrence and fate of selected surfactants in seawater at the outfall of the Marseille urban sewerage system. Int. J. Environ. Sci. Technol. 12, 1527–1538 (2015). https://doi.org/10.1007/s13762-014-0577-0

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s13762-014-0577-0

Keywords

Navigation