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Mercury cycling and species mass balances in four North American lakes
2009
Qureshi, Asif | Macleod, Matthew | Scheringer, Martin | Hungerbuhler, Konrad
A mass balance model for mercury based on the fugacity concept is applied to Lake Superior, Lake Michigan, Onondaga Lake and Little Rock Lake to evaluate model performance, analyze cycling of three mercury species groups (elemental, divalent and methyl mercury), and identify important processes that determine the source-to-concentration relationship of the three mercury species groups in these lakes. This model application to four disparate ecosystems is an extension of previous applications of fugacity-based models describing mercury cycling. The model performs satisfactorily following site-specific parameterization, and provides an estimate of minimum rates of species interconversion that compare well with literature. Volatilization and sediment burial are the main processes removing mercury from the lakes, and uncertainty analyses indicate that air-water exchange of elemental mercury and water–sediment exchange of divalent mercury attached to particles are influential in governing mercury concentrations in water. Any new model application or field campaign to quantify mercury cycling in a lake should consider these processes as important.
Show more [+] Less [-]Detection of phosphorus species in sediments of artificial landscape lakes in China by fractionation and phosphorus-31 nuclear magnetic resonance spectroscopy
2009
Liu, Jinyong | Wang, Hui | Yang, Haijun | Ma, Yanjun | Cai, Ouchen
Phosphorus (P) pollution in the sediments of seven artificial landscape lakes was studied via fractionation and phosphorus-31 nuclear magnetic resonance (31P NMR) spectroscopy. The lake sediments accumulated significant amounts of P from supplementation with reclaimed water and from runoff from the golf course lawns. The differences in total sediment P among lakes were correlated to the varied pollution extent from the lawns. One striking feature of the artificial lake sediments was the insufficiency of NaOH-extracted Al, which plays an important role in avoiding internal P release during anoxia. Another characteristic was the dominance of orthophosphate in the NaOH-EDTA extractants of the sediments, due to the heavy external P pollution. Phytate, considered prevalent in many soils and lake sediments, as well as polyphosphates and phosphonates which have appeared in some natural lake sediments, was not detected. The rank order of present biogenic P species was monoester-P > DNA-P > pyrophosphate > lipid-P. Mineral fixation and biological conversion of phosphorus were investigated in artificial lake sediments in China.
Show more [+] Less [-]Organochlorines in the Vaccarès Lagoon trophic web (Biosphere Reserve of Camargue, France)
2009
Roche, H. | Vollaire, Y. | Persic, A. | Buet, A. | Oliveira-Ribeiro, C. | Coulet, E. | Banas, D. | Ramade, F.
During a decade (1996-2006), ecotoxicological studies were carried out in biota of the Vaccarès Lagoon (Biosphere Reserve in Rhone Delta, France). A multicontamination was shown at all levels of the trophic web due to a direct bioconcentration of chemical from the medium combined with a food transfer. Here, the pollutants investigated were organochlorines, among which many compounds banned or in the course of prohibition (or restriction) (PCB, lindane, pp'-DDE, dieldrin, aldrin, heptachlor, endosulfan ...) and some substances likely still used in the Rhone River basin (diuron, fipronil). The results confirmed the ubiquity of contamination. It proves to be chronic, variable and tends to regress; however contamination levels depend on the trophic compartment. A biomagnification process was showed. A comparison of investigation methods used in other Mediterranean wetlands provides basis of discussion, and demonstrates the urgent need of modelling to assess the ecotoxicological risk in order to improve the management of such protected areas. The Vaccarès Lagoon trophic web biomagnifies organochlorine pollutants.
Show more [+] Less [-]Bioaccumulation of organochlorine pollutants in the fish community in Lake Årungen, Norway
2009
Sharma, Chhatra Mani | Rosseland, Bjørn Olav | Almvik, Marit | Eklo, Ole Martin
Organochlorine pollutants in the major fish species (pike Esox lucius, perch Perca fluviatilis, and roach Rutilus rutilus) of Lake Årungen, Norway, were investigated after an extensive removal of large pike in 2004. The organochlorine pollutants detected in fish liver samples in 2005 were dichlorodiphenyltrichloroethane (DDTs), polychlorinated biphenyls (PCBs), hexachlorobenzene (HCB), and heptachlor epoxide (HCE). DDTs were the dominant among all analyzed OCs. ΣPCB and HCB, detected in fish from two clearly distinct trophic levels (prey and predators), give an indication of biomagnification. All OC concentrations in female pike were significantly lower compared to males, which might be due to the removal of high concentrations of pollutants in roe during spawning. Organochlorine pollutants in fish tissues tend to magnify up the food chain.
Show more [+] Less [-]PCB accumulation in osprey exposed to local sources in lake sediment
2009
De Solla Shane R. | Martin, Pamela A.
We examined the accumulation of PCBs in ospreys (Pandion haleaetus) that were exposed to local sediment sources. Eggs, chick plasma, and sediment samples were collected over a range of 14 km (0.2-14.2 km) from a PCB source in Sturgeon Lake, ON. Sum PCB concentrations declined in chick plasma (range 422.5-58.3 ng/g) as distance from the PCB source increased, but there was a poor relationship with sum PCBs in eggs. Both tissues indicated an Aroclor 1248/1254 source. Aroclor 1254 comprised an average of 66.9% of sum PCBs in chick plasma from Sturgeon Lake, but comprised only from 27.0 to 44.4% in plasma from other Great Lake colonies. Dietary differences among osprey colonies were not sufficient to explain the PCB patterns observed. There was weak evidence that the ability to metabolize PCBs may differ between juveniles and adults, based upon the PCB profile in eggs and chick plasma. PCBs in plasma and eggs of osprey reflect local sources of PCBs in sediment.
Show more [+] Less [-]Dissecting the spatial scales of mercury accumulation in Ontario lake sediment
2009
Mills, R Brad | Paterson, Andrew M. | Lean, David R.S. | Smol, J. P. (John P) | Mierle, Greg | Blais, Jules M.
Total mercury concentration was analyzed in 171 lakes from pre-industrial (>30 cm depth; Hgpre-industrial) and present-day sediments (0.5-1 cm; Hgpresent-day). Numerous hot or cold spots of sediment mercury enrichment (Hg EF; Hgpre-industrial/Hgpresent-day) were evident as determined by local tests of autocorrelation, although in most cases, the maximum correlation among sites was not the nearest neighbor, indicating a strong influence of watershed characteristics. Hg EF was correlated with the area of open water (ha) (r = 0.91, p = 0.035), mine tailings (r = 0.94, p = 0.019), and organic deposits in surficial geology of the watershed (r = -0.91, p = 0.034). Through use of local rather than global regression coefficients, R2 increased from 0.20 (p = 0.005) to 0.60 (p = 0.013). A broad spatial pattern (>500 km) observed only in Hgpre-industrial was best explained by mean annual precipitation (shared variance = 3.5%), while finer spatial patterns only observed in Hgpresent-day and Hg EF were best explained by pH (average shared variance = 10.8%). Present mercury accumulation in lake sediment occurs on finer spatial gradients than found pre-industrially, these new spatial gradients correlate well with gradients in lake pH.
Show more [+] Less [-]PCBs in sediments of the Great Lakes - Distribution and trends, homolog and chlorine patterns, and in situ degradation
2009
Li, An | Rockne, Karl J. | Sturchio, Neil | Song, Wenlu | Ford, Justin C. | Wei, Hua
A region-wide data analysis on polychlorinated biphenyls (PCBs) in the sediment of the Great Lakes reveals a total accumulation of approximately 300 ± 50 tonnes, representing a >30% reduction from the 1980s. Evidence of in situ degradation of sediment PCB was found, with estimated t1/2 of 11 and 17 years, at two open water locations in Lake Ontario. The relative abundance of heavy homologs as well as para-chlorines decreases with increasing depth, while the opposite is true for medium and light homologs and ortho-chlorines. In Lake Michigan, the vertical pattern features enrichment of heavier congeners and reduction of ortho-chlorines in deeper sediment layers, opposite to the trend in Lake Ontario. PCBs decrease log-linearly with increasing latitude and longitude. Air deposition of PCBs to lake sediment decreases at about 0.077 ng cm-2 yr-1 per degree latitude (N) for the geographic region extending from the Great Lakes to within the Arctic Circle. Data analysis on PCBs in the Great Lakes sediments reveals decline of overall burden, occurrence of in situ degradation, and the geographic gradient in the region and beyond.
Show more [+] Less [-]Seasonal fluxes and temperature-dependent accumulation of persistent organic pollutants in lakes: The role of internal biogeochemical cycling
2009
Meijer, Sandra N. | Grimalt, Joan O. | Fernández, Pilar | Dachs, Jordi
A dynamic flux model for lakes taking into account the interactions between atmospheric depositional and biogeochemical processes (BIODEP model) was used to assess the importance of internal cycling and biogeochemical processes with respect to accumulation of four different polychlorinated biphenyls (PCBs) (congeners 28, 52, 101 and 153) in Lake Redo, a high-altitude lake in the Spanish Pyrenees. To investigate the effect of temperature on sediment accumulation, the model was run at different temperatures and corresponding sediment inventories were plotted vs. reciprocal temperature. In line with measurements from a previous study looking at sediment inventories of 19 European high-altitude lakes (MOLAR study), we found a stronger temperature dependence of lake sediment concentrations for the less volatile/less soluble PCBs. Seasonal and annual mass balances were investigated and highlighted the importance of internal lake processes controlling the differences in sediment accumulation for the different PCB congeners. For example, the higher temperature dependence of sediment inventories for the high chlorinated congeners is due to the fast dynamics of water-to-sediment transport in comparison to atmospheric deposition processes. A dynamic flux model was used to assess the importance of internal lake processes in controlling sediment accumulation for different PCB congeners.
Show more [+] Less [-]Sediment processes and mercury transport in a frozen freshwater fluvial lake (Lake St. Louis, QC, Canada)
2009
Canário, João | Poissant, Laurier | O'Driscoll, Nelson | Vale, Carlos | Pilote, Martin | Lean, D. R. S. (David R. S)
An open-bottom and a closed-bottom mesocosm were developed to investigate the release of mercury from sediments to the water column in a frozen freshwater lake. The mesoscosms were deployed in a hole in the ice and particulate mercury (HgP) and total dissolved mercury (TDHg) were measured in sediments and in water column vertical profiles. In addition, dissolved gaseous mercury (DGM) in water and mercury water/airflux were quantified. Concentrations of TDHg, DGM, and mercury flux were all higher in the open-bottom mesocosm than in the closed-bottom mesocosm. In this paper we focus on the molecular diffusion of mercury from the sediment in comparison with the TDHg accumulation in the water column. We conclude that the molecular diffusion and sediment resuspension play a minor role in mercury release from sediments suggesting that solute release during ebullition is an important transport process for mercury in the lake. In a frozen lake Hg is released from contaminated sediments mainly due to gas ebullition and molecular diffusion plays a minor role.
Show more [+] Less [-]Organic phosphorus species in surface sediments of a large, shallow, eutrophic lake, Lake Taihu, China
2009
Bai, Xiuling | Ding, Shiming | Fan, Chengxin | Liu, Tao | Shi, Dan | Zhang, Lu
Organic phosphorus (P) fractions in surface sediments from a large shallow, eutrophic Lake Taihu, China, were extracted with 0.1 M NaOH after pre-treatment of the sediments with a solution composed of 0.1 M EDTA and 2% (w/v) Na₂S₂O₄. Composition of organic P in the extracts was then characterized by ³¹P nuclear magnetic resonance spectroscopy (³¹P NMR). Several P species, including phosphonates, orthophosphate, orthophosphate monoesters, phospholipids, DNA, pyrophosphate and polyphosphate, were detected in the NaOH extracts. The proportion of extracted organic P to total P in sediments was negatively correlated with total P in the water column, as were the proportions for orthophosphate monoesters and DNA. This implies that the majority of organic P in surface sediments is likely stabilized in some way, and does not directly contribute to the internal loading of P from sediments. Organic phosphorus species in surface sediments of Lake Taihu.
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