| 1. |
- Chen, Long, et al.
(författare)
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A decline in Arctic Ocean mercury suggested by differences in decadal trends of atmospheric mercury between the Arctic and northern midlatitudes
- 2015
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Ingår i: Geophysical Research Letters. - 0094-8276 .- 1944-8007. ; 42:14, s. 6076-6083
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric mercury (Hg) in the Arctic shows much weaker or insignificant annual declines relative to northern midlatitudes over the past decade (2000-2009) but with strong seasonality in trends. We use a global ocean-atmosphere model of Hg (GEOS-Chem) to simulate these observed trends and determine the driving environmental variables. The atmospheric decline at northern midlatitudes can largely be explained by decreasing North Atlantic oceanic evasion. The midlatitude atmospheric signal propagates to the Arctic but is countered by rapid Arctic warming and declining sea ice, which suppresses deposition and promotes oceanic evasion over the Arctic Ocean. The resulting simulation implies a decline of Hg in the Arctic surface ocean that we estimate to be -0.67%yr(-1) over the study period. Rapid Arctic warming and declining sea ice are projected for future decades and would drive a sustained decline in Arctic Ocean Hg, potentially alleviating the methylmercury exposure risk for northern populations.
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| 2. |
- Kim, Hyunji, et al.
(författare)
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Methylmercury Mass Budgets and Distribution Characteristics in the Western Pacific Ocean
- 2017
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 51:3, s. 1186-1194
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Tidskriftsartikel (refereegranskat)abstract
- Methylmercury (MeHg) accumulation in marine organisms poses serious ecosystem and human health risk, yet the sources of MeHg in the surface and subsurface ocean remain uncertain. Here, we report the first MeHg mass budgets for the Western Pacific Ocean estimated based on cruise observations. We found the major net source of MeHg in surface water to be vertical diffusion from the subsurface layer (1.8-12 nmol m(-2) yr(-1)). A higher upward diffusion in the North Pacific (12 nmol m(-2) yr(-1)) than in the Equatorial Pacific (1.8-5.7 nmol m(-2) yr(-1)) caused elevated surface MeHg concentrations observed in the North Pacific. We furthermore found that the slope of the linear regression line for MeHg versus apparent oxygen utilization in the Equatorial Pacific was about 2-fold higher than that in the North Pacific. We suggest this could be explained by redistribution of surface water in the tropical convergence-divergence zone, supporting active organic carbon decomposition in the Equatorial Pacific Ocean. On the basis of this study, we predict oceanic regions with high organic carbon remineralization to have enhanced MeHg concentrations in both surface and subsurface waters.
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| 3. |
- Mason, Robert P., et al.
(författare)
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The Global Marine Selenium Cycle : Insights From Measurements and Modeling
- 2018
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Ingår i: Global Biogeochemical Cycles. - 0886-6236 .- 1944-9224. ; 32:12, s. 1720-1737
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Tidskriftsartikel (refereegranskat)abstract
- Anthropogenic activities have increased the selenium (Se) concentration in the biosphere, but the overall impact on the ocean has not been examined. While Se is an essential nutrient for microorganisms, there is little information on the impact of biological processes on the concentration and speciation of Se in the ocean. Additionally, other factors controlling the distribution and concentration of Se species are poorly understood. Here we present data gathered in the subtropical Pacific Ocean during a cruise in 2011, and we used these field data and the literature, as well as laboratory photochemical experiments examining the stability and degradation of inorganic Se (both Se (IV) and Se (VI)) and dimethyl selenide, to further constrain the cycling of Se in the upper ocean. We also developed a multibox model for the biosphere to examine the impact of anthropogenic emissions on the concentration and distribution of Se in the ocean. The model concurs with the field data indicating that the Se concentration has increased in the upper ocean waters over the past 30 years. Our observational studies and model results suggest that Se (VI) is taken up by phytoplankton in the surface ocean, in contrast to the results of laboratory culture experiments. In conclusion, while anthropogenic inputs have markedly increased Se in the atmosphere (42%) and net deposition to the ocean (38%) and terrestrial landscape (41%), the impact on Se in the ocean is small (3% increase in the upper ocean). This minimal response reflects its long marine residence time. Plain Language Summary We measured selenium in water and particles during a cruise in the Pacific Ocean and use this data along with laboratory photochemcial experiments to examine the formation and degradation of the various Se forms in the upper ocean. We also developed a box model to examine how anthropogenic activities have changed the Se concentration throughout the ocean the potential future impacts and to highlight areas of Se biogeochemistry that need further study.
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| 4. |
- Skrobonja, Aleksandra, 1990-
(författare)
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Formation, uptake and bioaccumulation of methylmercury in coastal seas : a baltic sea case study
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Methylmercury (MeHg) is a potent neurotoxin which can bioaccumulate to harmful levels in aquatic food webs. Methylmercury formation is a predominantly biotic process which involves phylogenically diverse microorganisms (e.g. iron- or sulfate-reducing bacteria). The formation of MeHg is related to the presence of organic matter (OM) which contains substrates essential for methylating microbes and reduced sulfur ligands (thiols, RSH) that form strong bonds with inorganic mercury (HgII) and affect its bioavailability. In aquatic systems, MeHg is bio-concentrated from the water column to the base of the food web and this step is crucial for MeHg levels found at higher trophic levels. Trophic transfer processes of MeHg in the food web are also of great importance. Discharge of OM in coastal areas affects light conditions needed for phytoplankton growth, and promotes heterotrophy, i.e. bacteria production. This may lead to a shift from the phytoplankton-based to the longer bacteria-based (microbial loop) food web and influence the amount of bioaccumulated MeHg in higher trophic levels. Methylmercury levels in predatory biota is thus affected by the bioavailability of HgII for methylation (studied in Paper I & II), MeHg speciation in the water column, crucial for MeHg incorporation at the base of the food web (Paper III), and the structure of the pelagic food web (Paper IV).In this thesis, it is shown that OM can act as a predictor of dissolved MeHg levels in estuarine and coastal systems. It impacts MeHg levels both by affecting HgII bioavailability (through Hg complexation with humic matter) and the activity of methylating microbes (providing metabolic electron donors) (Paper I). Moreover, elevated concentrations of particulate and dissolved HgII and MeHg, are associated with the presence of pelagic redoxclines in coastal seas. The redoxcline affects HgII speciation in the water column and its bioavailability for methylation (Paper II). It is further shown that the molecular structure of ligands in MeHg complexes affects the kinetics of MeHg uptake in phytoplankton. Rate constants for association of MeHg to the cell surface of a green algae were higher in treatments containing smaller thiol ligands of simpler structure than in treatments with larger thiols and more “branched” structure (Paper III). Finally, it is demonstrated that MeHg bioaccumulation in zooplankton can increase in systems with highly heterotrophic food webs and enhanced loadings of terrestrial OM (Paper IV). Such conditions are expected to occur in northern latitude coastal systems following climate changes.
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| 5. |
- Skrobonja, Aleksandra, et al.
(författare)
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Uptake Kinetics of Methylmercury in a Freshwater Alga Exposed to Methylmercury Complexes with Environmentally Relevant Thiols
- 2019
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 53:23, s. 13757-13766
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Tidskriftsartikel (refereegranskat)abstract
- Cellular uptake of dissolved methylmercury (MeHg) by phytoplankton is the most important point of entry for MeHg into aquatic food webs. However, the process is not fully understood. In this study we investigated the influence of chemical speciation on rate constants for MeHg accumulation by the freshwater green microalga Selenastrum capricornutum. We used six MeHg-thiol complexes with moderate but important structural differences commonly found in the environment. Rate constants for MeHg interactions with cells were determined for the MeHg-thiol treatments and a control assay containing the thermodynamically less stable MeHg0H complex. We found both elevated amounts of MeHg associated with whole cells and higher MeHg association rate constants in the control compared to the thiol treatments. Furthermore, the association rate constants were lower when algae were exposed to MeHg complexes with thiols of larger size and more branched chemical structure compared to complexes with simpler structure. The results further demonstrated that the thermodynamic stability and chemical structure of MeHg complexes in the medium is an important controlling factor for the rate of MeHg interactions with the cell surface, but not for the MeHg exchange rate across the membrane. Our results are in line with uptake mechanisms involving formation of MeHg complexes with cell surface ligands prior to internalization.
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| 6. |
- Soerensen, Anne L., et al.
(författare)
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A mass budget for mercury and methylmercury in the Arctic Ocean
- 2016
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Ingår i: Global Biogeochemical Cycles. - 0886-6236 .- 1944-9224. ; 30:4, s. 560-575
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Tidskriftsartikel (refereegranskat)abstract
- Elevated biological concentrations of methylmercury (MeHg), a bioaccumulative neurotoxin, are observed throughout the Arctic Ocean, but major sources and degradation pathways in seawater are not well understood. We develop a mass budget for mercury species in the Arctic Ocean based on available data since 2004 and discuss implications and uncertainties. Our calculations show that high total mercury (Hg) in Arctic seawater relative to other basins reflect large freshwater inputs and sea ice cover that inhibits losses through evasion. We find that most net MeHg production (20Mga(-1)) occurs in the subsurface ocean (20-200m). There it is converted to dimethylmercury (Me2Hg: 17Mga(-1)), which diffuses to the polar mixed layer and evades to the atmosphere (14Mga(-1)). Me2Hg has a short atmospheric lifetime and rapidly degrades back to MeHg. We postulate that most evaded Me2Hg is redeposited as MeHg and that atmospheric deposition is the largest net MeHg source (8Mga(-1)) to the biologically productive surface ocean. MeHg concentrations in Arctic Ocean seawater are elevated compared to lower latitudes. Riverine MeHg inputs account for approximately 15% of inputs to the surface ocean (2.5Mga(-1)) but greater importance in the future is likely given increasing freshwater discharges and permafrost melt. This may offset potential declines driven by increasing evasion from ice-free surface waters. Geochemical model simulations illustrate that for the most biologically relevant regions of the ocean, regulatory actions that decrease Hg inputs have the capacity to rapidly affect aquatic Hg concentrations.
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| 7. |
- Soerensen, Anne L., et al.
(författare)
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Deciphering the Role of Water Column Redoxclines on Methylmercury Cycling Using Speciation Modeling and Observations From the Baltic Sea
- 2018
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Ingår i: Global Biogeochemical Cycles. - : American Geophysical Union (AGU). - 0886-6236 .- 1944-9224. ; 32:10, s. 1498-1513
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Tidskriftsartikel (refereegranskat)abstract
- Oxygen-depleted areas are spreading in coastal and offshore waters worldwide, but the implication for production and bioaccumulation of neurotoxic methylmercury (MeHg) is uncertain. We combined observations from six cruises in the Baltic Sea with speciation modeling and incubation experiments to gain insights into mercury (Hg) dynamics in oxygen depleted systems. We then developed a conceptual model describing the main drivers of Hg speciation, fluxes, and transformations in water columns with steep redox gradients. MeHg concentrations were 2-6 and 30-55 times higher in hypoxic and anoxic than in normoxic water, respectively, while only 1-3 and 1-2 times higher for total Hg (THg). We systematically detected divalent inorganic Hg (Hg-II) methylation in anoxic water but rarely in other waters. In anoxic water, high concentrations of dissolved sulfide cause formation of dissolved species of Hg-II: HgS2H(aq)- and Hg (SH)(2)(0)((aq)). This prolongs the lifetime and increases the reservoir of Hg-II readily available for methylation, driving the high MeHg concentrations in anoxic zones. In the hypoxic zone and at the hypoxic-anoxic interface, Hg concentrations, partitioning, and speciation are all highly dynamic due to processes linked to the iron and sulfur cycles. This causes a large variability in bioavailability of Hg, and thereby MeHg concentrations, in these zones. We find that zooplankton in the summertime are exposed to 2-6 times higher MeHg concentrations in hypoxic than in normoxic water. The current spread of hypoxic zones in coastal systems worldwide could thus cause an increase in the MeHg exposure of food webs.
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| 8. |
- Soerensen, Anne. L., et al.
(författare)
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Eutrophication Increases Phytoplankton Methylmercury Concentrations in a Coastal Sea-A Baltic Sea Case Study
- 2016
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 50:21, s. 11787-11796
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Tidskriftsartikel (refereegranskat)abstract
- Eutrophication is expanding worldwide, but its implication for production and bioaccumulation of neurotoxic monomethylmercury (MeHg) is unknown. We developed a mercury (Hg) biogeochemical model for the Baltic Sea and used it to investigate the impact of eutrophication on phytoplankton MeHg concentrations. For model evaluation, we measured total methylated Hg (MeHgT) in the Baltic Sea and found low concentrations (39 +/- 16 fM) above the halocline and high concentrations in anoxic waters (1249 +/- 369 fM). To close the Baltic Sea MeHgT budget, we inferred an average normoxic water column HgII methylation rate constant of 2 x 10-4 d-1. We used the model to compare Baltic Seas present-day (2005-2014) eutrophic state to an oligo/mesotrophic scenario. Eutrophication increases primary production and export of organic matter and associated Hg to the sediment effectively removing Hg from the active biogeochemical cycle; this results in a 27% lower present-day water column Hg reservoir. However, increase in organic matter production and remineralization stimulates microbial Hg methylation resulting in a seasonal increase in both water and phytoplankton MeHg reservoirs above the halocline. Previous studies of systems dominated by external MeHg sources or benthic production found eutrophication to decrease MeHg levels in plankton. This Baltic Sea study shows that in systems with MeHg production in the normoxic water column eutrophication can increase phytoplankton MeHg content.
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| 9. |
- Soerensen, Anne Laerke, et al.
(författare)
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Organic matter drives high interannual variability in methylmercury concentrations in a subarctic coastal sea
- 2017
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Ingår i: Environmental Pollution. - : Elsevier. - 0269-7491 .- 1873-6424. ; 229, s. 531-538
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Tidskriftsartikel (refereegranskat)abstract
- Levels of neurotoxic methylmercury (MeHg) in phytoplankton are strongly associated with water MeHg concentrations. Because uptake by phytoplankton is the first and largest step of bioaccumulation in aquatic food webs many studies have investigated factors driving seasonal changes in water MeHg concentrations. Organic matter (OM) is widely accepted as an important driver of MeHg production and uptake by phytoplankton but is also known for strong interannual variability in concentration and composition within systems. In this study, we explore the role of OM on spatial and interannual variability of MeHg in a subarctic coastal sea, the northern Baltic Sea. Using MeHg (2014: 80 ± 25 fM; 2015: in situ MeHg production in the water column occurs during OM remineralization. The negative association between water humic content and MeHg concentration is most likely due to humic matter decreasing inorganic mercury (HgII) bioavailability to methylating microbes. With these relationships, we develop a statistical model and use it to calculate MeHg concentrations in late summer nearshore and offshore waters between 2006 and 2016 using measured values for water DOC and humic matter content. We find that MeHg concentrations can vary by up to an order of magnitude between years, highlighting the importance of considering interannual variability in water column MeHg concentrations when interpreting both short and long term MeHg trends in biota.
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| 10. |
- Song, S., et al.
(författare)
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Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling
- 2015
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:12, s. 7103-7125
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Tidskriftsartikel (refereegranskat)abstract
- We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg-0 observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations and also matches regional over-water Hg-0 and wet deposition measurements. The optimized global mercury emission to the atmosphere is 5.8 Gg yr(-1). The ocean accounts for 3.2 Gg yr(-1) (55 % of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg-0. The optimized Asian anthropogenic emission of Hg-0 (gas elemental mercury) is 650-1770 Mg yr(-1), higher than its bottom-up estimates (550-800 Mg yr(-1)). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23 % of present-day atmospheric deposition.
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