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Analysis of mud crab hepatopancreas proved to be a useful ap-proach for monitoring persistent organics and this study revealedresidual concentrations of DDTs and dieldrin in several northQueensland catchments two decades after deregistration. Whilepassive samplers were superior for monitoring current pesticides(Kapernick et al., 2006), mud crabs provided better evidence ofresidual OC contamination, and the data here provides an exten-sive baseline along the GBR for future comparison. The presenceof POCs such as DDTs and dieldrin was clearly related to urbaninfluences and the gradual degradation of POCs is likely to resultin further decreases in the body burdens of these contaminantsin tropical crabs in the future.
Acknowledgements
The Reef Water Quality Protection Plan Marine Monitoring Pro-gram was developed and run by the Great Barrier Reef Marine ParkAuthority on behalf of a consortium of research partners, includingthe Australian Institute of Marine Science, and funded by the Nat-ural Heritage Trust. The Authors also thank S. Boyle for the metalanalyses and A. Muirhead and G. Milton for valuable technicalassistance. EnTox is a partnership between Queensland Healthand the University of Queensland.
Appendix A. Supplementary data
Supplementary data associated with this article can be found, inthe online version, at doi:10.1016/j.marpolbul.2009.03.004.
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de Keyser, F., Lucas, K.G., 1968. Geology of the Hodgkinson and Laura Basins, NorthQueensland. Bureau of Mineral Resources, Australia Bulletin 84, 254p.
GBRMPA, 2001a. Great Barrier Reef Catchment Water Quality Action Plan: A Reportto Ministerial Council on Targets for Pollutant Loads. Great Barrier Reef MarinePark Authority, Townsville.
GBRMPA, 2001b. Population and Major Land Use in the Great Barrier ReefCatchment Area: Spatial and Temporal Trends. Great Barrier Reef Marine ParkAuthority, Townsville.
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Haynes, D., Johnson, J.E., 2000. Organochlorine, heavy metal and polyaromatichydrocarbon pollutant concentrations in the Great Barrier Reef (Australia)environment: a review. Marine Pollution Bulletin 41, 267–278.
Haynes, D., Muller, J., Carter, S., 2000. Pesticide and herbicide residues in sedimentsand seagrasses from the Great Barrier Reef World Heritage Area andQueensland Coast. Marine Pollution Bulletin 41, 279–287.
Haynes, D., Müller, J.F., McLachlan, M.S., 1999. Polychlorinated dibenzo-p-dioxinsand dibenzofurans in great barrier reef (Australia) dugongs (Dugong dugon).Chemosphere 38, 255–262.
Humphrey, C.A., Codi King, S., Klumpp, D.W., 2007. A multibiomarker approach inbarramundi (Lates calcarifer) to measure exposure to contaminants in estuariesof tropical North Queensland. Marine Pollution Bulletin 54, 1569–1581.
Kapernick, A., Shaw, M., Dunn, A., Komarova, T., Müller, J., Carter, S., Eaglesham, G.,Schaffelke, B., Bass, D., Haynes, D., 2006. River pesticide loads and GBR lagoonpesticide data. In: Schaffelke, B., Waterhouse, J. (Eds.), Water Quality andEcosystem Monitoring Program – Reef Water Quality Protection Plan. FinalReport August 2006. Report to the Great Barrier Reef Marine Park Authority.CRC Reef Research Consortium, Townsville, pp. 66–104.
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0025-326X/$ - see front matter Crown Copyright � 2009 Published by Elsevier Ltd. All rights reserved.doi:10.1016/j.marpolbul.2009.03.004
Levels and spatial distribution of polychlorinated biphenyls (PCBs) insuperficial sediment from 15 Italian Marine Protected Areas (MPA)
Karla Pozo *, Denise Lazzerini, Guido Perra, Valerio Volpi, Simonetta Corsolini, Silvano FocardiEnvironmental Science Department, University of Siena, Via Mattioli 4, 53100 Siena, Italy
Human activities such as industry, sewage, coastal sprawl,intensive agriculture and oil spills have a high impact on the Med-iterranean marine environment. In Italy, growing awareness ofhow man is threatening marine ecosystems has prompted conser-vation measures, including the designation of Marine Protected
Areas (MPAs). MPAs are essential for conservation, providing pro-tection for critical areas and refuges for overexploited species. Theycan also act as buffers against management miscelation (Allisonet al., 1998). Italy has instituted a number of MPAs that are provingeffective in protecting wildlife. Most of them contain one or moreno-entry zones which coincide with the areas of greatest naturalvalue (Boero et al., 1999). However, MPAs cannot protect popula-tions or assemblages from transboundary movements of chemicals
* Corresponding author. Tel.: +39 0577232879; fax: +39 0577232806.E-mail address: [email protected] (K. Pozo).
Baseline / Marine Pollution Bulletin 58 (2009) 765–786 773
(I.U.C.N, 1981), a phenomenon observed mostly in MPAs locatednear human activities such as harbours. MPAs can be useful formonitoring release of contaminants. For instance, Terlizzi et al.(2004) reported the effects of organotin compounds such as tribu-tyltin (TBT) and its transboundary movements in species of marinesnails living in Italian MPAs.
Persistent organic pollutants (POPs) are semivolatile organiccompounds of special concern because of their toxicity, persis-tence, long-range transport and bioaccumulation potential (UNEP,2001). POPs such as polychlorinated biphenyls (PCBs) have beenwidely used in industry and are characterized by low vapour pres-sure, low water solubility and environmental persistence (Mackayet al., 1992). Since they are hydrophobic they bind readily to par-ticulate in water and are transported/deposited with sediment intorivers, lakes and oceans (Bergamaschi et al., 2001). The StockholmConvention on POPs, coordinated through the United NationsEnvironment Programme (UNEP), aims to reduce or eliminate theuse, discharge and emission of these compounds to the benefit ofthe environment, reducing risks to humans and wildlife (UNEP,2001). Initially, 12 chemicals were identified as priority POPs: nineorganochlorine pesticides (OCPs), one industrial chemical class,polychlorinated biphenyls (PCBs) and polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs) associated with various indus-trial/combustion emissions (UNEP, 2001). Several countries in Eur-ope are parties to the Convention; Italy signed the StockholmConvention in May 2001, but has not yet ratified it.
PCBs were widely used as insulating fluids in electrical equip-ment, such as transformers and capacitors, and for many other
uses. Italian production of PCBs began in 1958. PCB mixtures wereproduced by Caffaro S.p.A. under different names, including Apiro-lio and Fenchlor. Production was estimated at 6000 ton in 1970–1974; in the same period 13,000 ton of PCBs were imported fromFrance (Prodelec), Germany (Bayer) and USA (Monsanto). The mix-tures most frequently imported from the USA were aroclor 1254and 1260 (35:65). Although use of PCBs was banned in Italy in1984 (Ruzzenenti, 2003), there is only fragmented, discontinuousdata for POP levels in Italian marine environments. Sampling withbetter spatial resolution is required to assess the spatial/temporaltrends, levels and fate of PCBs in Italy. The aim of this study wasto obtain information on spatial distribution of PCB levels in super-ficial sediments from 15 MPAs.
Superficial sediment samples were collected by scuba divingfrom no-access zones of 15 Italian MPAs (Fig. 1) during June to Au-gust 2001. Sediment samples consisted mainly of coarse and med-ium sand. Latitude, longitude and depth of each sampling sites arelisted in Table 1. Samples were transported to the laboratory in anice cooler where they were weighed and sealed to avoid contami-nation. Sediment samples (5–10 g) were freeze dried at �50 �C and0.2 mbars and homogenised with anhydrous sodium sulphate.They were then extracted three times with 50 ml n-hexane:dichlo-romethane (DCM) (1:1) in an ultrasonic bath for 20 min and centri-fuged at 1500 rpm to separate sediment from solvent extract. Finalsolvent extracts (150 ml) were concentrated to 5 ml in a rotaryevaporator and percolated through activated copper to remove sul-phur. The extracts were reduced to about 0.5 ml and charged on asilica gel column activated at 130 �C overnight. The silica column
Fig. 1. Mean PCB concentrations (a) and homologue composition (%) (b) in sediments from 15 Italian Marine Protected Areas.
774 Baseline / Marine Pollution Bulletin 58 (2009) 765–786
was slurry packed with hexane. The PCB fraction was eluted with33.5 ml hexane:DCM (1:1) and blown down with nitrogen (Cousinsand Jones, 1998).
PCBs were analysed by gas chromatography using a Perkin El-mer Autosystem gas chromatograph fitted with a 63Ni electroncapture detector. GC conditions are described in Pozo et al.(2007). PCBs were quantified using Arochlor 1260 mixture fromSupelco Inc. (USA) as external standard. All compounds were ana-lytical standards of >99% purity. The standard mix contained 36congeners (Table 1). Detection limits using GC-ECD were approxi-mately 0.05 ng ml�1 for most individual components based oninjection of 1.0 ll and assuming a signal-to-noise ratio > 3. Theabove procedures were checked for recoveries and reproducibility.Procedural blanks and reference material (purchased from Na-tional Institute of Standards and Technology (NIST)) were analysedfor quality assurance and quality control (QA/QC) purposes. Detailsof recovery tests and analytical blanks were reported by Pozo et al.(2007). PCB concentrations were adjusted by subtracting blank val-ues and expressed in ng g�1 on a dry weight (d.w.) basis. Organiccarbon (OC) percentage (%) was also analysed. Details of samplepreparation and clean up are described elsewhere (Pozo et al.,2007). Statistical analysis was carried out using SAS Version 5 soft-ware. The Pearson correlation was used to analyse relationshipsbetween PCBs and organic carbon percentage (%).
Table 1 shows mean concentrations of PCBs and organic carbon%. Total PCB concentrations decreased in the following order: Mir-amare > Punta Campanella > Isole Tremiti > Cinque Terre > CapoRizzuto > Portofino > Isola di Santo Stefano > Torre Guaceto > CapoCarbonara > Isole Egadi > Porto Cesareo > Isola di Ustica > Isola diTavolara > Isole Ciclopi > Peninsola Sinis (with levels below detec-tion limit) (Fig. 1a). Thus PCBs were detected in fourteen of the15 MPAs considered. With the exception of Miramare, mean PCBconcentrations (ng g�1 d.w.) were low and ranged from 0.1 ± 0.1(at Isole Ciclopi, easthern Sicily) to 4 ± 8 (Punta Campanella, southwest Italy). These results are similar to those reported by Tolosaet al. (1995) in superficial sediments from the Mediterranean be-tween the Balearic islands and Corsica (2–3 ng g�1 d.w.) and withbackground levels established by Gomez-Gutiérrez et al. (2007)(1–5 ng g�1). The highest PCB levels (84 ± 112) were detected atMiramare, northern Adriatic sea (Fig. 1a). These concentrationsare in line with those reported in other Italian marine coastal areas(Table 2). The data in Table 2 demonstrates that PCB levels at Mir-amare are linked to a local ‘‘hot spot” caused by nearby industrialplants, shipping and sewage disposal. The Miramare sampling siteis in a sheltered bay and with limited water exchange, enhancingthe accumulation of pollutants.
PCB homologue composition analysis showed three differenthomologue patterns. Tetra-Cl (congeners PCB-70 + 76), detectedin southern Italy, was the predominant PCB homologue group,accounting for 40–48% of total PCB composition (at Punta Campa-nella, Isole Ciclopi, Isole Egadi, Porto Cesareo, Isola di Tavolara, Iso-la di Ustica) (Fig. 1b). The second group, detected at most of thesites, showed a prevalence of middle-to-highly chlorinated PCBs,with hexa-Cl (PCB-149, �153, �138) accounting for 48–52% of to-tal PCB composition (at Cinque Terre, Porto Fino, Torre Guaceto,Capo Carbonara, Capo Rizzuto and Isole Tremiti). In the thirdgroup, detected in northern Italy (Miramare), hepta-Cl (PCB-170,180) accounted for 44% of total PCB composition (Fig. 1b). For Isoladi S. Stefano, central Italy, no clear PCB composition was observed.These PCB patterns are the result of weathering effect which isassociated with degradation under different environmental condi-tions. In some cases, weathering may actually heighten toxicity be-cause less completely chlorinated molecules lose chlorine atomsfirst, leaving the more highly chlorinated and more toxic moleculesbehind (National Research Council, 2001). This effect was evidentin most MPAs, especially Miramare, as most PCB patterns weredominated by moderately to highly chlorinated PCBs. Organic car-bon percentages were low, ranging from 0.3% (Capo Rizzuto) to 2%(Punta Campanella) (Table 1). Pearson correlation analysis did notshow any statistical correlation between organic carbon (%) andPCB concentrations (p < 0.05).
In conclusion, these results provide information on the currentstatus of Italian MPAs. PCB concentrations were low at most sitesand consistent with background levels reported in previous stud-ies, with the exception of Miramare adjacent the port of Trieste.At the Miramare site, PCB concentrations were closely related tolocal ‘‘hot spot” because the industrial and port activities.
The low concentrations and PCB pattern detected in most of theMPAs (except at Miramare) suggest that the main sources areatmospheric deposition rather than nearby human activities. These
Table 1Mean concentrations of PCBs (ng g�1 d.w) and OC percentage (%) in 15 Italian MPAs. Location of sampling sites and depth are also shown.
Location MPA Zone A Latitude Longitude Depth (m) Samples (n=) OC (%) aMean PCBs SD
North east Miramare Castello di Miramare 45�4201100N 13�4204300 E �5 6 0,9 84 112North west Cinque Terre Punta Mesco 44�0806100N 09�3702600E �15 6 0,4 2 2North west Portofino Cala dell’Oro (‘‘Punta del Buco”) 44�1804400N 09�1000000E �16 6 0,3 1 0,4Center Isola Santo Stefano Isoloto Santo Stefano 40�4704000N 13�2704700E �20 6 0,5 0,3 0,3Central east Isole Tremiti Isola di Pianosa 2�1304200N 15�44030‘‘ E �29 6 0,5 2 4South west Punta Campanella Scoglio Vervece 40�3704200N 14�1906600E �20 6 2 4 8South Torre Guaceto Isoloto Canale Reale 40�4204400N 17�4803500E �3 6 0,9 0,3 0,1South Porto Cesareo Frascone 40�1200400N 17�5502100E �3 6 0,6 0,2 0,2South Capo Rizzuto Capo Cimiti 38�5609900N 17�0906600E �6 4 0,3 2 1,5Sardinia Isola Tavolara Isola di Molara 40�5207600N 09�4306400E �4 6 0,8 0,1 0,1Sardinia Capo Carbonara Isola di Serpentara 39�0708300N 09�3604300E �4 6 0,5 0,3 0,3Sardinia P.del Sinis Torre del Sevo 39�5400000N 08�2400200E �6 6 0,6 BDL naSicily Isole Ciclopi Faraglioni 37�3304200N 15�1000300E �15 4 0,3 0,1 0,1Sicily Isole Egadi Isola di Marettimo (‘‘Punta Libeccio”) 37�5704200N 12�0204600E �7 8 0,3 0,2 0,2Sicily Isola Ustica Cala Sidoti 38�4201200N 13�0901800E �6 6 0,3 0,1 0,1
Abbreviations: SD, standard deviation; m, meters; n, number; na, not available; BDL, below detection limit; MDL, method detection limit (<0.05 ng g�1).a RPCB represented by the following IUPAC congeners = 3-Cl: 70 + 76, 60 + 56; 5-Cl: 95, 101, 105, 110; 6-Cl: 151, 144 + 135, 118 + 149, 134, 146, 141, 153, 137, 138, 158,
128; 7-Cl: 176, 178, 187, 183, 185, 174, 177, 171 + 202, 172, 180, 189, 170; 8-Cl: 199, 196, 201, 195, 194, 205.
Table 2PCB concentrations (ng g�1 d.w.) in sediments from other Italian marine coastal areas.
Sites ng g�1 dw References
Northern Adriatic 3.2–58 Burns and Villeneuve (1983)Lagoon of Venice 6–1590 Frignani et al. (2001)Mar Piccolo Taranto 2–1684 Cardellicchio et al. (2007)Lagoon of Venice 185 Raccanelli et al. (1989)Lagoon of Venice 128–180 Pavoni et al. (1990)Gulf of Triestea 293 ± 120 Adami et al. (2000)
a Sampling site located near the Miramare site used in the present study.
Baseline / Marine Pollution Bulletin 58 (2009) 765–786 775
results can be used as baseline for further monitoring programsand for planning better strategies to protect Italian MPAs. How-ever, a better understanding of the effectiveness of MPAs and theimpacts of chemicals on marine biodiversity is needed.
Acknowledgements
Financial support of the AFRODITE project. We thank the projectco-ordinators, R. Cattaneo-Vietti and S. Greco, and the regional col-laborators: S. Bava, P. Addis, M. Murenu, S. Bussotti and R. Chem-ello who helped to obtain sediment samples from various MPAs.
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Allison, G.W., Lubchenco, J., Carr, M.H., 1998. Marine reserve are necessary but notsufficient for marine conservation. Ecol. Appl. 8, 79–92.
Bergamaschi, B.A., Kuivia, K.M., Fram, M.S., 2001. Pesticides associated withsuspended sediments entering San Francisco Bay following the first majorstorm of water year 1996. Estuaries. 24, 368–380.
Boero, F., Brian, F., Micheli, F., 1999. Scientific Design and Monitoring ofMediterranean Marine Protected Areas. CIESM Workshop Series 8, pp. 64.
Burns, K.A., Villeneuve, J.P., 1983. Biogeochemical processes affecting thedistribution and vertical transport of hydrocarbons residues in the coastalMediterranean. Geochim. Cosmochim. Acta 47, 995–1006.
Cardellicchio, N., Buccolieri, A., Giandomenico, S., Lopez, L., Pizzulli, F., Spada, L.,2007. Organic pollutants (PAHs, PCBs) in sediments from the Mar Piccolo inTaranto (Ionian Sea, Southern Italy). Mar. Pollut. Bull 55, 451–458.
Cousins, I.T., Jones, K.C., 1998. Air–soil exchange of semi-volatile organiccompounds (SOCs) in the UK. Environ. Pollut. 102, 105–118.
Frignani, M., Belluci, L.G., Carrar, C., Raccanelli, S., 2001. Polychlorinated biphenylsin sediments of the Venice Lagoon. Chemosphere 43, 567–575.
Gomez-Gutiérrez, A., Garnacho, E., Bayona, J.M., Albaigés, J., 2007. Assessment of theMediterranean sediment contamination by persistent organic pollutants.Environ. Pollut. 148, 396–408.
I.U.C.N., 1981. Principles, criteria and guidelines for the selection establishment andmanagement of Mediterranean marine and costal protected areas. Gland, CH.
Mackay, D., Shiu, W.Y., Ma, K.C., 1992. Illustrated Handbook of Physical–Chemical,vol. I. Monoaromatic Hydrocarbons, Chlorobenzenes and PCBs (also vol. II, 1992,and vol. III, 1993). Lewis Publishers, Chelsea, MI, 697 pp.
National Research Council, Committee on Remediation of PCB-ContaminatedSediments. A Risk-Management Strategy for PCB-Contaminated Sediments.National Academy Press, Washington, DC, 2001.
Pavoni, B., Calvo, C., Sfrisio, A., Orio, A.A., 1990. Time trend of PCB concentrations insurface sediment from a hypertrophic, macroalgae populated area of the lagoonof Venice. Sci. Tot. Environ. 91, 13–21.
Pozo, K., Urrutia, R., Barra, R., Mariottini, M., Treutler, H.C., Araneda, A., Focardi, S.,2007. Records of polychlorinated biphenyls (PCBs) in sediments of four remoteChilean Andean Lakes. Chemosphere 66, 1911–1921.
Raccanelli, S., Pavoni, B., Marcomini, A., Orio, A.A., 1989. Polychlorinated biphenylpollution caused by resuspension of surface sediments in the lagoon of Venice.Sci. Tot. Environ. 79, 11–123.
Ruzzenenti, M., 2003. La storia dei PCB (Policlorobifenili). Miracoli e disastri dellatecnica del novecento. Saggio. Altronovecento. Ambiente-Tecnica-Società.Rivista on-line promossa da Fondazione ‘‘Luigi Micheletti” di Brescia. 2003,No. 6-febbraio. <(www.altronovecento.quipo.it)>.
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0025-326X/$ - see front matter � 2009 Elsevier Ltd. All rights reserved.doi:10.1016/j.marpolbul.2009.03.003
Assessment of soft-bottom Polychaeta assemblage affected by a spatialconfluence of impacts: Sewage and brine discharges
Del-Pilar-Ruso Yoana *, De-la-Ossa-Carretero Jose Antonio, Loya-Fernández Angel,Ferrero-Vicente Luis Miguel, Giménez-Casalduero Francisca, Sánchez-Lizaso Jose LuisDpto. de Ciencias del Mar y Biología Aplicada. Universidad de Alicante. Campus de San Vicente del Raspeig, Ap. 99, E-03080 Alicante, Spain
Mediterranean coastal areas are subject to significant pressurescaused by human activity. Sewage effluent is considered one of themost common anthropogenic disturbances of marine benthic com-munities and it has long been recognized as one of the principalcauses of faunal change in near-shore benthic environments (Pear-son and Rosenberg, 1978; Lercari and Defeo, 2003), and it can alsolead to severe habitat degradation in marine environments (Hunterand Evans, 1995). There is a considerable body of knowledge oftemporal and spatial benthic population and community dynamicsin relation to certain types of disturbance, especially organicenrichment (Pearson and Rosenberg, 1978; Rhoads and Germano,1986; Cardell et al., 1999).
In recent years a new activity has appeared that may affectcoastal areas: seawater desalination plants. In the Mediterranean,the total production of fresh water from seawater is about 4.2 mil-lion m3/day (17% of the worldwide production). Spain, with 7%, isthe largest producer in the region and about 70% of the Spanish
plants are located on the Mediterranean coast (Lattemann andHöpner, 2008), and most of these employ reverse osmosis technol-ogy. The introduction of a desalination plant will inevitably beassociated with several potential adverse environmental impactsparticularly on marine ecosystems (Alameddine and El-Fabel,2007). The main impact on marine communities of reverse osmosisdesalination plants is caused by the discharge of an effluent of veryhigh salinity (70–90 psu). The magnitude of the impact will dependboth on the size of the plant and on the sensitivity of the ecosystemthat receives the spill (Höpner and Windelberg, 1996). However, itmay mainly affect marine benthic communities due to the highdensity of the brine discharge which remains on the bottom.
In addition, there is the increasing possibility that benthic com-munities will feel the impact of both sewage outfall and brine dis-charge when and wherever these processes merge. Growingpressure on the coastal zone has increased the number of large-scale, diffuse and chronic impacts operating on coastal and estua-rine ecosystems. Multiple sources and types of impacts interactingover a range of spatial scales complicate the assessment and man-agement of such ecosystems (Hewitt et al., 2005).
* Corresponding author. Tel.: +34 965 90 34 00x2916; fax: +34 965 90 98 40.E-mail address: [email protected] (Del-Pilar-Ruso Yoana).
776 Baseline / Marine Pollution Bulletin 58 (2009) 765–786