Occurrence of pharmaceuticals and endocrine disrupting compounds in macroalgaes, bivalves, and fish from coastal areas in Europe.

The occurrence and levels of PhACs, Endocrine Disrupting and related Compounds (EDCs) in seafood from potential contaminated areas in Europe has been studied. Macroalgae (Saccharina latissima and Laminaria digitata), bivalves (Mytilus galloprovincialis, Mytilus spp., Chamalea gallina and Crassostrea gigas) and fish (Liza aurata and Platichthys flesus) from Portugal, Spain, Italy, Netherlands, and Norway were analysed following 4 different analytical protocols depending on the organism and target group of contaminants. The results revealed the presence of 4 pharmaceutical compounds in macroalgae samples, 16 in bivalves and 10 in fish. To the best of our knowledge, this is the first time that PhACs have been detected in marine fish and in macroalgae. Besides, this is also the first time that dimetridazole, hydrochlorothiazide and tamsulosin have been detected in biota samples. The highest levels of PhACs corresponded to the psychiatric drug velanfaxine (up to 36.1 ng/g dry weight (dw)) and the antibiotic azithromycin (up to 13.3 ng/g dw) in bivalves from the Po delta (Italy). EDCs were not detected in macroalgae samples, however, the analysis revealed the presence of 10 EDCs in bivalves and 8 in fish. The highest levels corresponded to the organophosphorus flame retardant tris(2-butoxyethyl)phosphate (TBEP) reaching up to 98.4 ng/g dw in mullet fish from the Tagus estuary. Bivalves, in particular mussels, have shown to be good bioindicator organisms for PhACs and fish for EDCs. Taking into consideration the concentrations and frequencies of detection of PhACs and EDCs in the seafood samples analysed, a list of candidates' compounds for priorization in future studies has been proposed.

[1]  Åke Bergman,et al.  State of the Science of Endocrine Disrupting Chemicals - 2012 , 2012 .

[2]  D. Barceló,et al.  The occurrence of polybrominated diphenyl ethers in river and coastal biota from Portugal. , 2006, Chemosphere.

[3]  K. Kannan,et al.  Occurrence of and dietary exposure to parabens in foodstuffs from the United States. , 2013, Environmental science & technology.

[4]  B. Paull,et al.  A year-long study of the spatial occurrence and relative distribution of pharmaceutical residues in sewage effluent, receiving marine waters and marine bivalves. , 2014, The Science of the total environment.

[5]  E. Ballesteros,et al.  Determination of residual pharmaceuticals in edible animal tissues by continuous solid-phase extraction and gas chromatography-mass spectrometry. , 2011, Talanta.

[6]  Colin R. Janssen,et al.  Development of analytical strategies using U-HPLC-MS/MS and LC-ToF-MS for the quantification of micropollutants in marine organisms , 2011, Analytical and bioanalytical chemistry.

[7]  S. Tanabe,et al.  Simultaneous determination of polar pharmaceuticals and personal care products in biological organs and tissues. , 2014, Journal of chromatography. A.

[8]  F. Cabello,et al.  Heavy use of prophylactic antibiotics in aquaculture: a growing problem for human and animal health and for the environment. , 2006, Environmental microbiology.

[9]  Peter Haglund,et al.  Organophosphorus flame retardants and plasticizers in marine and fresh water biota and in human milk. , 2010, Journal of environmental monitoring : JEM.

[10]  Joon-Woo Kim,et al.  Multiresidue analytical method for the determination of antimicrobials, preservatives, benzotriazole UV stabilizers, flame retardants and plasticizers in fish using ultra high performance liquid chromatography coupled with tandem mass spectrometry. , 2011, Journal of chromatography. A.

[11]  M. Servos,et al.  Antidepressants and their metabolites in municipal wastewater, and downstream exposure in an urban watershed , 2010, Environmental toxicology and chemistry.

[12]  C. Casellas,et al.  Occurrence of venlafaxine residues and its metabolites in marine mussels at trace levels: development of analytical method and a monitoring program , 2013, Analytical and Bioanalytical Chemistry.

[13]  Enzo Funari,et al.  Alkylphenols and their ethoxylates in seafood from the Tyrrhenian Sea. , 2008, Chemosphere.

[14]  D. Voutsa,et al.  Occurrence and partitioning of endocrine-disrupting compounds in the marine environment of Thermaikos Gulf, Northern Aegean Sea, Greece. , 2012, Marine pollution bulletin.

[15]  M Gros,et al.  Analysis of multi-class pharmaceuticals in fish tissues by ultra-high-performance liquid chromatography tandem mass spectrometry. , 2013, Journal of chromatography. A.

[16]  C. Chambliss,et al.  Bioaccumulation and trophic dilution of human pharmaceuticals across trophic positions of an effluent-dependent wadeable stream , 2014, Philosophical Transactions of the Royal Society B: Biological Sciences.

[17]  K. Thomas,et al.  Sources, impacts and trends of pharmaceuticals in the marine and coastal environment , 2014, Philosophical Transactions of the Royal Society B: Biological Sciences.

[18]  D. Barceló,et al.  Multi-residue method for the analysis of pharmaceuticals and some of their metabolites in bivalves. , 2015, Talanta.

[19]  G. Pojana,et al.  Natural and synthetic endocrine disrupting compounds (EDCs) in water, sediment and biota of a coastal lagoon. , 2007, Environment international.

[20]  S. Bayen,et al.  Occurrence and distribution of pharmaceutically active and endocrine disrupting compounds in Singapore's marine environment: influence of hydrodynamics and physical-chemical properties. , 2013, Environmental pollution.

[21]  D. Voutsa,et al.  Polar organic micropollutants in the coastal environment of different marine systems. , 2014, Marine pollution bulletin.

[22]  Duane B Huggett,et al.  Field and laboratory fish tissue accumulation of the anti-convulsant drug carbamazepine. , 2012, Ecotoxicology and environmental safety.

[23]  A. Gallipoli,et al.  Exposure of the Main Italian River Basin to Pharmaceuticals , 2011, Journal of toxicology.

[24]  D. Barceló,et al.  Development of a liquid chromatography-tandem mass spectrometry procedure for determination of endocrine disrupting compounds in fish from Mediterranean rivers. , 2013, Journal of chromatography. A.

[25]  M. Campos,et al.  Current status and perspectives of mollusc (bivalves and gastropods) culture in the Spanish Mediterranean , 2005 .

[26]  J. Pawliszyn,et al.  Optimization of solid phase microextraction for non-lethal in vivo determination of selected pharmaceuticals in fish muscle using liquid chromatography-mass spectrometry. , 2012, Journal of chromatography. A.

[27]  A. Sapkota,et al.  Aquaculture practices and potential human health risks: current knowledge and future priorities. , 2008, Environment international.

[28]  G. Ying,et al.  Steroids in marine aquaculture farms surrounding Hailing Island, South China: occurrence, bioconcentration, and human dietary exposure. , 2015, The Science of the total environment.

[29]  D. Barceló,et al.  Seasonal distribution of pharmaceuticals in marine water and sediment from a Mediterranean coastal lagoon (SE Spain). , 2015, Environmental research.

[30]  J. Gelsleichter,et al.  Uptake of human pharmaceuticals in bull sharks (Carcharhinus leucas) inhabiting a wastewater-impacted river. , 2013, The Science of the total environment.

[31]  Alejandro J. Ramirez,et al.  Analysis of pharmaceuticals in fish using liquid chromatography-tandem mass spectrometry. , 2007, Analytical chemistry.

[32]  Gianmarco Giordani,et al.  The Sacca di Goro Lagoon and an Arm of the Po River , 2006 .

[33]  M. L. La Guardia,et al.  Occurrence of contaminants of emerging concern in mussels (Mytilus spp.) along the California coast and the influence of land use, storm water discharge, and treated wastewater effluent. , 2014, Marine pollution bulletin.

[34]  D. Barceló,et al.  Risk assessment based prioritization of 200 organic micropollutants in 4 Iberian rivers. , 2015, The Science of the total environment.

[35]  C. Casellas,et al.  Fast and easy extraction combined with high resolution-mass spectrometry for residue analysis of two anticonvulsants and their transformation products in marine mussels. , 2013, Journal of chromatography. A.

[36]  Richard Grace,et al.  Method validation and reconnaissance of pharmaceuticals, personal care products, and alkylphenols in surface waters, sediments, and mussels in an urban estuary. , 2013, Environment international.

[37]  Lingxin Chen,et al.  Occurrence of parabens in foodstuffs from China and its implications for human dietary exposure. , 2013, Environment international.

[38]  C. Delerue-Matos,et al.  Assessment of non-steroidal anti-inflammatory and analgesic pharmaceuticals in seawaters of North of Portugal: occurrence and environmental risk. , 2015, The Science of the total environment.

[39]  J. Sumpter.  Feminized responses in fish to environmental estrogens. , 1995, Toxicology letters.

[40]  H. Neels,et al.  Brominated flame retardants and polychlorinated biphenyls in fish from the river Scheldt, Belgium. , 2008, Environment international.

[41]  D. Barceló,et al.  Determination of a broad spectrum of pharmaceuticals and endocrine disruptors in biofilm from a waste water treatment plant-impacted river. , 2016, The Science of the total environment.

[42]  Yaqi Cai,et al.  Investigation of antibiotics in mollusks from coastal waters in the Bohai Sea of China. , 2012, Environmental pollution.

[43]  D. Podlipna,et al.  Determination of bisphenol A in canned fish by sol–gel immunoaffinity chromatography, HPLC and fluorescence detection , 2007 .

[44]  S. Bay,et al.  Organic contaminants of emerging concern in sediments and flatfish collected near outfalls discharging treated wastewater effluent to the Southern California Bight , 2012, Environmental toxicology and chemistry.