Despite the fact that most persistent toxic substances have hardly been primarily emitted for several decades, their concentrations are only slowly decreasing in the global oceans. Surface seawater samples were collected along a 38°-24° N/28°-67° W transect in the subtropical North Atlantic Ocean. While the concentration levels of hexachlorobenzene (2.1-6.1 pg L-1), dichlorodiphenyltrichloroethane (DDT, up to 2.1 pg L-1) and polychlorinated biphenyls (PCB, 10.8-24.9 pg L-1) were in the same range as observed earlier in the North Atlantic, hexachlorocyclohexane (HCH, 90-627 pg L-1) was found elevated, partly also relative to previous measurements in the same sea region. Hereby, the ratio α-HCH/γ-HCH was very low, 0.09-0.13. Chlordane and endosulfan were found in the range <3.0-11.1 and <5.8-8.8 pg L-1 respectively. DDT metabolites, endrin and related pesticides were found below quantification limits. Spatial pollution patterns in surface seawaters seem to be determined by atmospheric and oceanic transport patterns, rather than by mixing and air-sea equilibrium. The comparison with global multicompartment chemistry-transport model predictions of surface seawater levels indicate underestimated degradation of PCBs and overestimated emissions of endosulfan.

Centre for Earth System Research and Sustainability Institute for Geology University of Hamburg Hamburg Germany

Federal Maritime and Hydrographic Agency Hamburg Germany

Man Technology Environment Research Centre Örebro University Örebro Sweden

Max Planck Institute for Meteorology Hamburg Germany

Multiphase Chemistry Department Max Planck Institute for Chemistry Mainz Germany

Research Centre for Toxic Compounds in the Environment Masaryk University Brno Czech Republic

Zobrazit více v PubMed

Breivik K, Sweetman A, Pacyna JM, Jones KC. Towards a global historical emission inventory for selected PCB congeners—a mass balance approach. 3. An update. Sci Tot Environ. 2007;377:296–307. doi: 10.1016/j.scitotenv.2007.02.026. PubMed DOI

Cai MG, Qiu CR, Shen Y, Cai MH, Huang SY, Qian BH, Sun JH, Liu XY. Concentration and distribution of 17 organochlorine pesticides (OCPs) in seawater from the Japan Sea northward to the Arctic Ocean. Sci China Chem. 2010;53:1033–1047. doi: 10.1007/s11426-010-0182-0. DOI

Denier van der Gon H, van het Bolscher M, Visschedijk A, Zandveld P. Emissions of POPs and eight candidate POPs from UNECE-Europe in 2000, 2010 and 2020 and the emission reduction resulting from the implementation of the UNECE POP protocol. Atmos Environ. 2007;41:9245–9261. doi: 10.1016/j.atmosenv.2007.06.055. DOI

Gioia R, Nizzetto L, Lohmann R, Dachs J, Temme C, Jones KC. Polychlorinated biphenyls (PCBs) in air and seawater of the Atlantic Ocean: sources, trends and processes. Environ Sci Technol. 2008;42:1416–1422. doi: 10.1021/es071432d. PubMed DOI

Harvey GR, Steinhauer WG. Atmospheric transport of polychlorinated biphenyls to the North Atlantic. Atmos Environ. 1974;8:777–782. doi: 10.1016/0004-6981(74)90173-5. PubMed DOI

Hühnerfuss H, Faller J, König WA, Ludwig P. Gas-chromatographic separation of the the enantiomers of marine pollutants. 4. Fate of HCH isomers in the Baltic and North Sea. Environ Sci Technol. 1992;26:2127–2133. doi: 10.1021/es00035a009. DOI

Iwata H, Tanabe S, Sakai N, Tasukawa R. Distribution of persistent organochlorines in the oceanic air and surface seawater and the role of ocean on their global transport and fate. Environ Sci Technol. 1993;27:1080–1098. doi: 10.1021/es00043a007. DOI

Jakobi G, Kirchner M, Henkelmann B, Körner W, Offenthaler I, Moche W, Weiss P, Schaub M, Schramm KW. Atmospheric bulk deposition measurements of organochlorine pesticides at three alpine summits. Atmos Environ. 2015;101:158–165. doi: 10.1016/j.atmosenv.2014.10.060. DOI

Jantunen LMM, Bidleman TF. Reversal of the air-water gas-exchange direction of hexachlorocyclohexanes in the Bering and Chukchi seas: 1993 vs. 1988. Environ Sci Technol. 1995;29:1081–1089. doi: 10.1021/es00004a030. PubMed DOI

Jantunen LMM, Bidleman TF. Organochlorine pesticides and enantiomers of chiral pesticides in Arctic Ocean water. Arch Environ Contam Toxicol. 1998;35:218–228. doi: 10.1007/s002449900370. PubMed DOI

Jantunen LMM, Kylin H, Bidleman TF. Air–water gas exchange of α-hexachlorocyclohexane enantiomers in the South Atlantic Ocean and Antarctica. Deep Sea Res II. 2004;51:2662–2671. doi: 10.1016/j.dsr2.2004.02.002. DOI

Kunugi M, Abe S, Tsurukawa M, Matsumara C, Fujimori K, Nakano T (2010) Monitoring of the global scale pollution in seawater with persistent organic pollutants deployed on voluntary observation ships—monitoring on Pacific Ocean. Bunseki Kagaku 59:967–984

Lakaschus S, Weber K, Wania F, Schrems O. The air-sea equilibrium and time trend of hexachlorocyclohexanes in the Atlantic Ocean between the Arctic and Antarctica. Environ Sci Technol. 2002;36:138–145. doi: 10.1021/es010211j. PubMed DOI

Lammel G, Stemmler I. Fractionation and current time trends of PCB congeners: evolvement of distributions 1950–2010 studied using a global atmosphere-ocean general circulation model. Atmos Chem Phys. 2012;12:7199–7213. doi: 10.5194/acp-12-7199-2012. DOI

Li YF. Global technical hexachlorocyclohexane usage and its contamination consequences in the environment: from 1948 to 1997. Sci Total Environ. 1999;232:121–158. doi: 10.1016/S0048-9697(99)00114-X. DOI

Li NQ, Wania F, Lei YD, Daly GL. A comprehensive and critical compilation, evaluation, and selection of physicalchemical property data for selected polychlorinated biphenyls. J Phys Chem Ref Data. 2003;32:1545–1590. doi: 10.1063/1.1562632. DOI

Lohmann R, Muir D. Global aquatic passive sampling (AQUA-GAPS): using passive samplers to monitor POPs in the waters of the world. Environ Sci Technol. 2010;44:880–884. PubMed

Lohmann R, Breivik K, Dachs J, Muir D. Global fate of persistent organic pollutants: current and future research directions. Environ Pollut. 2007;150:150–165. doi: 10.1016/j.envpol.2007.06.051. PubMed DOI

Lohmann R, Gioia R, Jones KC, Nizzetto L, Temme C, Xie ZY, Schulz-Bull D, Hand I, Morgan E, Jantunen L. Organochlorine pesticides and PAHs in the surface water and atmosphere of the North Atlantic and Arctic Ocean. Environ Sci Technol. 2009;43:5633–5639. doi: 10.1021/es901229k. PubMed DOI

Lohmann R, Klánová J, Kukucka P, Yonis S, Bollinger K. PCBs and OCPs on a east-to-west transect: the importance of major currents and net volatilization for PCBs in the Atlantic Ocean. Environ Sci Technol. 2012;46:10471–14579. doi: 10.1021/es203459e. PubMed DOI

Magalhães MJ, de Barros MC. The contamination of fish with chlorinated hydrocarbons in Portugal: continental coast and Azores islands. Environ Mon Assess. 1987;8:37–57. doi: 10.1007/BF00396606. PubMed DOI

Mai C, Theobald N, Lammel G, Hühnerfuss H (2016) Persistent organochlorine pesticides and polychlorinated biphenyls in air of the North Sea region and air-sea exchange. Environ Sci Pollut Res, submitted manuscript PubMed PMC

Nizzetto L, Lohmann R, Gioia R, Dachs J, Jones KC. Atlantic Ocean surface waters buffer declining atmospheric concentrations of persistent organic pollutants. Environ Sci Technol. 2010;44:6978–6984. doi: 10.1021/es101293v. PubMed DOI

Octaviani M, Stemmler I, Lammel G, Graf HF. Atmospheric transport of persistent organic pollutants to and from the Arctic under present-day and future climate. Environ Sci Technol. 2015;49:3593–3602. doi: 10.1021/es505636g. PubMed DOI

Pontolillo J, Eganhouse RP (2001) The search for reliable aqueous solubility (Sw) and octanol-water partition coefficient (Kow) data for hydrophobic organic compounds: DDT and DDE as a case study, Tech. rep., U.S. Geological Survey, Water-Resource Investigations Report 01-4201, Reston, USA

Potter TL, Hapeman CJ, McConnell LL, Harman-Fetcho JA, Schmidt WF, Rice CP, Schaffer BA. Endosulfan wet deposition in Southern Florida (USA) Sci Total Environ. 2014;468:505–513. doi: 10.1016/j.scitotenv.2013.08.070. PubMed DOI

Qiu X, Zhu T, Yao B, Hu J, Hu S. Contribution of dicofol to the current DDT pollution in China. Environ Sci Technol. 2005;39:4385–4390. doi: 10.1021/es050342a. PubMed DOI

Rippen G (2008) Umweltchemikalien. Ecomed Publ, Landsber, Germany (CDROM ed.)

Roscales JL, Muñoz-Arnanz J, Lez-Solís JG, Jiménez B. Geographical PCB and DDT patterns in shearwaters (Calonectris sp.) breeding across the NE Atlantic and the Mediterranean archipelagos. Environ Sci Technol. 2010;44:2328–2334. doi: 10.1021/es902994y. PubMed DOI

Schulz-Bull DE, Petrick G, Bruhn R, Duinker JC. Chlorobiphenyls (PCB) and PAHs in water masses of the northern North Atlantic. Mar Chem. 1998;61:101–114. doi: 10.1016/S0304-4203(98)00010-3. DOI

Semeena VS, Lammel G. Effects of various scenarios upon entry of DDT and γ-HCH into the global environment on their fate as predicted by a multicompartment chemistry-transport model. Fresenius Environ Bull. 2003;12:925–939.

Shen L, Wania F. Compilation, evaluation, and selection of physical-chemical property data for organochlorine pesticides. J Chem Eng Data. 2005;50:742–768. doi: 10.1021/je049693f. DOI

Spencer WF, Cliath MM. Volatility of DDT and related compounds. J Agric Food Chem. 1972;20:645–649. doi: 10.1021/jf60181a057. PubMed DOI

Stemmler I, Lammel G. Cycling of DDT in the global oceans 1950–2002: World ocean returns the pollutant. Geophys Res Lett. 2009;36 doi: 10.1029/2009GL041340. DOI

Stemmler I, Lammel G. Evidence of the return of past pollution in the ocean—a model study. Geophys Res Lett. 2013;40:1373–1378. doi: 10.1002/grl.50248. DOI

UNEP (2003) Regionally based assessment of persistent toxic substances—global report. United Nations Environment Programme, Châtelaine, 207 pp

Wania F, Daly G. Estimating the contribution of degradation in air and deposition to the deep sea to the global loss of PCBs. Atmos Environ. 2002;36:5581–5593. doi: 10.1016/S1352-2310(02)00693-3. DOI

Walse SS, Scott GI, Ferry JL. Stereoselective degradation of aqueous endosulfan in modular estuarine mesocosms: formation of endosulfan γ-hydroxycarboxylate. J Environ Mon. 2003;5:373–379. doi: 10.1039/B212165D. PubMed DOI

Weber J, Halsall CJ, Muir DCG, Teixeira C, Small J, Solomon K, Hermanson M, Hung H, Bidleman T. Endosulfan, a global pesticide: a review of its fate in the environment and occurrence in the Arctic. Sci Total Environ. 2010;408:2966–2984. doi: 10.1016/j.scitotenv.2009.10.077. PubMed DOI

Xiao H, Li NQ, Wania F. Compilation, evaluation and selection of physic-chemical property data for σ-, β- and γ-HCH. J Chem Eng Data. 2004;49:173–185. doi: 10.1021/je034214i. DOI

Xie ZY, Koch BP, Möller A, Sturm R, Ebinghaus R. Transport and fate of hexachlorocyclohexanes in the oceanic air and surface seawater. Biogeosci. 2011;8:2621–2633. doi: 10.5194/bg-8-2621-2011. DOI

Yue Q, Zhang K, Zhang BZ, Li SM, Zeng EY. Occurrence, phase distribution and depositional intensity of dichlorodiphenyltrichloroethane (DDT) and its metabolites in air and precipitation of the Pearl River Delta, China. Chemosph. 2011;84:446–451. doi: 10.1016/j.chemosphere.2011.03.045. PubMed DOI

Zhong GC, Xie ZY, Cai MH, Möller A, Sturm R, Tang JH, Zhang G, He JF, Ebinghaus R. Distribution and air-sea exchange of current-use pesticides (CUPs) from East Asia to the high Arctic Ocean. Environ Sci Technol. 2012;47:259–267. doi: 10.1021/es202655k. PubMed DOI