Abstract
Concentrations and fluxes of total and methylmercury were determined in surface sediments and associated with settling particles at two sites in Lake Geneva to evaluate the sources and dynamics of this toxic contaminant. Total mercury concentrations measured in settling particles were different throughout the seasons and were greatly influenced by the Rhone River particulate inputs. Total mercury concentrations closer to shore (NG2) ranged between 0.073 ± 0.001 and 0.27 ± 0.01 μg/g, and between 0.038 ± 0.001 and 0.214 ± 0.008 μg/g at a site deeper in the lake (NG3). Total mercury fluxes ranged between 0.144 ± 0.002 and 3.0 ± 0.1 μg/m2/day at NG2, and between 0.102 ± 0.008 and 1.32 ± 0.08 μg/m2/day at NG3. Combined results of concentrations and fluxes showed that total mercury concentrations in settling particles are related to the season and particle inputs from the Rhone River. Despite an observed decrease in total mercury fluxes from the coastal zone towards the open lake, NG3 (~ 3 km from the shoreline) was still affected by the coastal boundary, as compared to distal sites at the center of the lake. Thus, sediment focusing is not efficient enough to redistribute contaminant inputs originating from the coastal zones, to the lake center. Methylmercury concentrations in settling particles largely exceeded the concentrations found in sediments, and their fluxes did not show significant differences with relation to the distance from shore. The methylmercury found associated with settling particles would be related to the lake’s internal production rather than the effect of transport from sediment resuspension.
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Baskaran M, Miller CJ, Kumar A, Andersen E, Hui J, Selegeanc JP, Creech CT, Barkach J (2015) Sediment accumulation rates and sediment dynamics using five different methods in a well-constrained impoundment: case study from union Lake, Michigan. J Great Lakes Res 41:607–617
Bengtsson G, Picado F (2008) Mercury sorption to sediments: dependence on grain size, dissolved organic carbon, and suspended bacteria. Chemosphere 73:526–531
Benoit JM, Gilmour CC, Mason RP, Riedel GS, Riedel GF (1998) Behavior of mercury in the Patuxent River estuary. Biogeochemistry 40:249–265
Blais JM, Kalff J (1995) The influence of lake morphometry on sediment focusing. Limnol Oceanogr 40:582–588
Bloesch J, Uehlinger U (1986) Horizontal sedimentation differences in a eutrophic Swiss Lake. Limnol Oceanogr 31:1094–1109
Bloom N (1989) Determination of Picogram levels of methylmercury by aqueous phase Ethylation, followed by cryogenic gas-chromatography with cold vapor atomic fluorescence detection. Can J Fish Aquat Sci 46:1131–1140
Bloom NS, Gill GA, Cappellino S, Dobbs C, Mcshea L, Driscoll C, Mason R, Rudd J (1999) Speciation and cycling of mercury in Lavaca Bay, Texas, sediments. Environ Sci Technol 33:7–13
Bravo AG, Bouchet S, Amouroux D, Poté J, Dominik J (2011) Distribution of mercury and organic matter in particle-size classes in sediments contaminated by a waste water treatment plant: Vidy Bay, Lake Geneva, Switzerland. J Environ Monit 13:974–982
Burnier G, Jaquerod CA, Poget E, Vioget P (2011) Bilans 2011 de l’épuration vaudoise. Rapport du service des eaux, sols et assaisnissement, Etat de Vaud, 27 pp
Compeau G, Bartha R (1984) Methylation and demethylation of mercury under controlled redox, Ph, and salinity conditions. Appl Environ Microbiol 48:1203–1207
Dean WE (1974) Determination of carbonate and organic matter in calcareous sediments and sedimentary rocks by loss on ignition; comparison with other methods. J Sediment Res 44:242–248
Dominik J, Burrus D, Vernet J-P (1987) Transport of the environmental radionuclides in an alpine watershed. Earth Planet Sci Lett 84:165–180
Dominik J, Dulinski M, Span D, Hofmann A, Favarger P-Y, Vernet J-P (1993) Transfert de matière et de radio-isotopes entre l'eau et les sédiments dans le Léman. Rapp Comm int prot eaux Léman contre pollut Campagne 1992:163–188
Drevnik PE, Shinneman ALC, Lamborg CH, Engstrom DR, Bother MH, Oris JT (2010) Mercury fluxes to sediments of Lake Tahoe, California-Nevada. Watet Air Soil Pollut 210:399–407
Ethier ALM, Atkinson JF, DePinto JV, Lean DRS (2012) Estimating mercury concentrations and fluxes in the water column and sediment of Lake Ontario with HERMES model. Environ Pollut 161:335–342
Evans RD (1994) Empirical-evidence of the importance of sediment resuspension in lakes. Hydrobiologia 284:5–12
Feyte S, Gobeil C, Tessier A, Cossa D (2012) Mercury dynamics in lake sediments. Geochim Cosmochim Acta 82:92–112
Fuchs A, Selmeczy GB, Kasprzak P, Padisák J, Casper P (2016) Coincidence of sedimentation peaks with diatom blooms, wind, and calcite precipitation measured in high resolution by a multi-trap. Hydrobiologia 763:329–344
Gagnon C, Pelletier E, Mucci A (1997) Behaviour of anthropogenic mercury in coastal marine sediments. Mar Chem 59:159–176
Gandais V (1989) Origines et variations spatio-temporelles des flux de matière particulaire au centre du Léman. Dissertation, University of Geneva
Gascón Díez E, Bravo AG, Porta AN, Masson M, Graham ND, Stoll S, Akhtman Y, Amouroux D, Loizeau J-L (2013) Influence of a wastewater treatment plant on mercury contamination and sediment characteristics in Vidy Bay (Lake Geneva, Switzerland). Aquat Sci 76:S21–S32
Gascón Díez E, Loizeau J-L, Cosio C, Bouchet S, Adatte T, Amouroux D, Bravo AG (2016) Role of settling particles on mercury methylation in the oxic water column of freshwater systems. Environ Sci Technol 50:11672–11679
Gascón Díez E, Corella JP, Adatte T, Thevenon F, Loizeau J-L (2017) High-resolution reconstruction of the 20th century history of trace metals, major elements, and organic matter in sediments in a contaminated area of Lake Geneva, Switzerland. Appl Geochem 78:1–11
Gilmour CC, Podar M, Bullock AL, Graham AM, Brown SD, Somenahally AC, Johs A, Hurt RA, Bailey KL, Elias DA (2013) Mercury methylation by novel microorganisms from new environments. Environ Sci Technol 47:11810–11820
Graham ND (2015) The fate of sediment-bound contaminants: a case study of Vidy Bay (Lake Geneva, Switzerland. Dissertation, University of Geneva
Graham ND, Bouffard D, Loizeau J-L (2016) The influence of bottom boundary layer hydrodynamics on sediment focusing in a contaminated bay. Environ Sci Pollut Res 23:25412–25426
Håkanson L (1977) The influence of wind, fetch, and water depth on the distribution of sediments in Lake Vänern, Sweden. Can J Earth Sci 14:397–412
Håkanson L, Jansson M (1983) Principles of lake sedimentology. Springer-Verlag, Berlin
Heimburger LE, Cossa D, Marty JC, Migon C, Averty B, Dufour A, Ras J (2010) Methyl mercury distributions in relation to the presence of nano- and picophytoplankton in an oceanic water column (Ligurian Sea, North-Western Mediterranean). Geochim Cosmochim Acta 74:5549–5559
Hurley JP, Watras CJ, Bloom NS (1991) Mercury cycling in a northern Wisconsin seepage lake: the role of particulate matter in vertical transport. Water Air Soil Pollut 56:543–551
Kim EH, Mason RP, Porter ET, Soulen HL (2006) The impact of resuspension on sediment mercury dynamics, and methylmercury production and fate: a mesocosm study. Mar Chem 102:300–315
Kocman D, Wilson SJ, Amos HM, Telmer KH, Steenhuisen F, Sunderland EM, Mason RP, Outridge P, Horvat M (2017) Toward an assessment of the global inventory of present-day mercury releases to freshwater environments. Int J Environ Res Public Health 14:138
Korthals ET, Winfrey MR (1987) Seasonal and spatial variations in mercury methylation and demethylation in an oligotrophic Lake. Appl Environ Microbiol 53:2397–2404
Liu B, Yan HY, Wang CP, Li QH, Guedron S, Spangenberg JE, Feng XB, Dominik J (2012) Insights into low fish mercury bioaccumulation in a mercury-contaminated reservoir, Guizhou, China. Environ Pollut 160:109–117
Loizeau J-L, Arbouille D, Santiago S, Vernet J-P (1994) Evaluation of a wide-range laser diffraction grain-size analyzer for use with sediments. Sedimentology 41:353–361
Loizeau J-L, Girardclos S, Dominik J (2012) Taux d'accumulation de sédiments récents et bilan de la matière particulaire dans le Léman (Suisse - France). Arch Sci 65:81–92
Loizeau J-L, Makri S, Arpagaus P, Ferrari B, Casado-Martinez C, Benejam T, Marchand P (2017) Micropolluants métalliques et organiques dans les sédiments superficiels du Léman. Rapp Comm int prot eaux Léman contre pollut Campagne 2016:143–198
Marvin C, Charlton M, Milne J, Thiessen L, Schachtschneider G, Sverko E (2007) Metals associated with suspended sediments in lakes Erie and Ontario, 2000-2002. Environ Monit Assess 130:149–161
Mason RP, Kim EH, Cornwell J, Heyes D (2006) An examination of the factors influencing the flux of mercury, methylmercury and other constituents from estuarine sediment. Mar Chem 102:96–110
Mason RP, Choi AL, Fitzgerald WF, Hammerschmidt CR, Lamborg CH, Soerensen AL, Sunderland EM (2012) Mercury biogeochemical cycling in the ocean and policy implications. Environ Res 119:101–117
OFEV (Editor) (2016) Annuaire hydrologique de la Suisse 2010. Office fédéral de l’environnement, Berne. Etat de l’environnement n° 1631: 627
Pardos M, Benninghoff C, De Alencastro LF, Wildi W (2004) The impact of a sewage treatment plant’s effluent on sediment quality in a small bay in Lake Geneva (Switzerland–France). Part 1: spatial distribution of contaminants and the potential for biological impacts. Lakes Reserv Res Manag 9:41–52
Parks JM, Johs A, Podar M, Bridou R, Hurt RA, Smith SD, Tomanicek SJ, Qian Y, Brown SD, Brandt CC, Palumbo AV, Smith JC, Wall JD, Elias DA, Liang LY (2013) The genetic basis for bacterial mercury methylation. Science 339:1332–1335
Podar M, Gilmour CC, Brandt CC, Soren A, Brown SD, Crable BR, Palumbo AV, Somenahally AC, Elias DA (2015) Global prevalence and distribution of genes and microorganisms involved in mercury methylation. Sci Adv 1(9):e1500675
Poté J, Haller L, Loizeau J-L, Bravo AG, Sastre V, Wildi W (2008) Effects of a sewage treatment plant outlet pipe extension on the distribution of contaminants in the sediments of the bay of Vidy, Lake Geneva, Switzerland. Bioresour Technol 99:7122–7131
Razmi AM, Barry DA, Bakhtyar R, Le Dantec N, Dastgheib A, Lemin U, Wüest A (2013) Current variability in a wide and open lacustrine embayment in Lake Geneva (Switzerland). J Great Lakes Res 39:455–465
Rigaud S, Radakovitch O, Couture RM, Deflandre B, Cossa D, Garnier C, Garnier JM (2013) Mobility and fluxes of trace elements and nutrients at the sediment-water interface of a lagoon under contrasting water column oxygenation conditions. Appl Geochem 31:35–51
Rolfhus KR, Sakamoto HE, Cleckner LB, Stoor RW, Babiarz CL, Back RC, Manolopoulos H, Hurley JP (2003) Distribution and fluxes of total and methylmercury in Lake superior. Environ Sci Technol 37:865–872
Roos-Barraclough F, Shotyk W (2003) Millennial-scale records of atmospheric mercury deposition obtained from ombrotrophic and minerotrophic peatlands in the Swiss Jura Mountains. Environ Sci Technol 37:235–244
Roos-Barraclough F, Givelet N, Martinez-Cortizas A, Goodsite ME, Biester H, Shotyk W (2002) An analytical protocol for the determination of total mercury concentrations in solid peat samples. Sci Total Environ 292:129–139
Savoye L, Quetin P, Klein A (2015) Physico-chemical changes in the waters of Lake Geneva. Meteorological datas Contributions from the tributaries of Lake Geneva and from the Rhone below Geneva. Rapp Comm int prot eaux Léman contre pollut Campagne 2014:19–67
Schartup AT, Ndu U, Balcom PH, Mason RP, Sunderland EM (2015) Contrasting effects of marine and terrestrially derived dissolved organic matter on mercury speciation and bioavailability in seawater. Environ Sci Technol 49:5965–5972
Taylor SE, Birch GF (2000) Contaminant dynamics in offchannel embayments of port Jackson, new South Wales. AGSO 5-6:233–237
Thevenon F, Graham ND, Chiaradia M, Arpagaus P, Wildi W, Poté J (2011) Local to regional scale industrial heavy metal pollution recorded in sediments of large freshwater lakes in Central Europe (lakes Geneva and Lucerne) over the last centuries. Sci Total Environ 412:239–247
Van Metre PC (2011) Increased atmospheric deposition of mercury in reference lakes near major urban areas. Environ Pollut 162:209–215
Wang WX, Stupakoff I, Gagnon C, Fisher NS (1998) Bioavailability of inorganic and methylmercury to a marine deposit feeding polychaete. Environ Sci Technol 32:2564–2571
Wiklund JA, Kirk JL, Muir DCG, Evans M, Yang F, Keating J, Parsons MT (2017) Anthropogenic mercury deposition in Flin Flon Manitoba and the Experimental Lakes area Ontario (Canada): a multi-lake sediment core reconstruction. Sci Total Environ 586:685–695
Acknowledgements
We would like to thank Philippe Arpagaus for his help during the sampling campaigns, in addition to “La Direction Générale de l’Environnement DGE–Inspection de la pêche” and “Canton de Vaud” for allowing us to deploy the sediment traps in Lake Geneva. The work was partially funded by SNF research grant PDFMP2-123034.
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Díez, E.G., Graham, N.D. & Loizeau, JL. Total and methyl-mercury seasonal particulate fluxes in the water column of a large lake (Lake Geneva, Switzerland). Environ Sci Pollut Res 25, 21086–21096 (2018). https://doi.org/10.1007/s11356-018-2252-3
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DOI: https://doi.org/10.1007/s11356-018-2252-3