177 research outputs found

    Mercury in tundra vegetation of Alaska: Spatial and temporal dynamics and stable isotope patterns

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    Vegetation uptake of atmospheric mercury (Hg) is an important mechanism enhancing atmospheric Hg deposition via litterfall and senescence. We here report Hg concentration and pool sizes of different plant functional groups and plant species across nine tundra sites in northern Alaska. Significant spatial differences were observed in bulk vegetation Hg concentrations at Toolik Field station (52 ± 9 μg kg−1), Eight Mile Lake Observatory (40 ± 0.2 μg kg−1), and seven sites along a transect from Toolik Field station to the Arctic coast (36 ± 9 μg kg−1). Hg concentrations in non-vascular vegetation including feather and peat moss (58 ± 6 μg kg−1 and 34 ± 2 μg kg−1, respectively) and brown and white lichen (41 ± 2 μg kg−1 and 34 ± 2 μg kg−1, respectively), were three to six times those of vascular plant tissues (8 ± 1 μg kg−1 in dwarf birch leaves and 9 ± 1 μg kg−1 in tussock grass). A high representation of nonvascular vegetation in aboveground biomass resulted in substantial Hg mass contained in tundra aboveground vegetation (29 μg m−2), which fell within the range of foliar Hg mass estimated for forests in the United States (15 to 45 μg m−2) in spite of much shorter growing seasons. Hg stable isotope signatures of different plant species showed that atmospheric Hg(0) was the dominant source of Hg to tundra vegetation. Mass-dependent isotope signatures (δ202Hg) in vegetation relative to atmospheric Hg(0) showed pronounced shifts towards lower values, consistent with previously reported isotopic fractionation during foliar uptake of Hg(0). Mass-independent isotope signatures (Δ199Hg) of lichen were more positive relative to atmospheric Hg(0), indicating either photochemical reduction of Hg(II) or contributions of inorganic Hg(II) from atmospheric deposition and/or dust. Δ199Hg and Δ200Hg values in vascular plant species were similar to atmospheric Hg(0) suggesting that overall photochemical reduction and subsequent re-emission was relatively insignificant in these tundra ecosystems, in agreement with previous Hg(0) ecosystem flux measurements

    Comment on “The biosphere: A homogeniser of Pb-isotope signals” by C. Reimann, B. Flem, A. Arnoldussen, P. Englmaier, T.E. Finne, F. Koller and Ø. Nordgulen

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    Reimann et al. (2008) recently published a study on Pb-isotope signature along a 120 km long transect cutting the city of Oslo. Based on concentration but also isotope data, they misinterpret Pb concentration of the biosphere in rural places and explain these large enrichments of Pb as being due to natural processes. The study ignores numerous previous studies either on local, regional or global scales (see reviews by Shotyk and Le Roux, 2005 and Callender, 2003, and references therein), which clearly demonstrate that anthropogenic Pb emitted in the atmosphere from different sources (leaded gasoline, coal burning, metallurgy, etc.) was and is dispersed worldwide. The study also ignores work on Norway by the Steinnes and colleagues group (Harmens et al., 2008, Steinnes et al., 2005a, Steinnes et al., 2005b and Åberg et al., 2004), and measurements and modelling by the EMEP network (www.emep.int/, EMEP, 2005). The study also neglects numerous works on preanthropogenic Pb deposition rate and isotopic signature using continental archives of atmospheric deposition like peat bogs (Shotyk et al., 1998, Klaminder et al., 2003, Kylander et al., 2005 and Le Roux et al., 2005). These studies have shown that preanthropogenic Pb atmospheric deposition rate and its Pb isotopic signature is regionally defined, but also that those signals are negligible compared to past 2 ka and recent Pb atmospheric fluxes (Table 1)

    Automated Stable Isotope Sampling of Gaseous Elemental Mercury (ISO-GEM): Insights into GEM Emissions from Building Surfaces

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    Atmospheric monitoring networks quantify gaseous elemental mercury (GEM) concentrations, but not isotopic compositions. Here, we present a new method for automated and quantitative stable isotope sampling of GEM (ISO-GEM) at the outlet of a commercial Hg analyzer. A programmable multivalve manifold selects Hg at the analyzer inlet and outlet based on specific criteria (location, time, GEM concentration, auxiliary threshold). Outlet Hg recovery was tested for gold traps, oxidizing acidic solution traps, and activated carbon traps. We illustrate the ISO-GEM method in an exploratory study on the effect of building walls on local GEM. We find that GEM concentrations directly at the building surface (wall inlet) are significantly enhanced (mean 3.8 ± 1.8 ng/m; 3; ) compared to 3 m from the building wall (free inlet) (mean 1.5 ± 0.4 ng/m; 3; ). GEM δ; 202; Hg (-1.26‰ ± 0.41‰, 1 SD, n = 16) and Δ; 199; Hg (-0.05‰ ± 0.10‰, 1 SD, n = 16) at the wall inlet were different from ambient GEM δ; 202; Hg (0.76‰ ± 0.09‰, 1 SD, n = 16) and Δ; 199; Hg (-0.21‰ ± 0.05‰, 1 SD, n = 16) at the free inlet. The isotopic fingerprint of GEM at the wall inlet suggests that GEM emission from the aluminum building surface affected local GEM concentration measurements. These results illustrate the versatility of the automated Hg isotope sampling

    Examination of the ocean as a source for atmospheric microplastics

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    Global plastic litter pollution has been increasing alongside demand since plastic products gained commercial popularity in the 1930’s. Current plastic pollutant research has generally assumed that once plastics enter the ocean they are there to stay, retained permanently within the ocean currents, biota or sediment until eventual deposition on the sea floor or become washed up onto the beach. In contrast to this, we suggest it appears that some plastic particles could be leaving the sea and entering the atmosphere along with sea salt, bacteria, virus’ and algae. This occurs via the process of bubble burst ejection and wave action, for example from strong wind or sea state turbulence. In this manuscript we review evidence from the existing literature which is relevant to this theory and follow this with a pilot study which analyses microplastics (MP) in sea spray. Here we show first evidence of MP particles, analysed by μRaman, in marine boundary layer air samples on the French Atlantic coast during both onshore (average of 2.9MP/m3) and offshore (average of 9.6MP/m3) winds. Notably, during sampling, the convergence of sea breeze meant our samples were dominated by sea spray, increasing our capacity to sample MPs if they were released from the sea. Our results indicate a potential for MPs to be released from the marine environment into the atmosphere by sea-spray giving a globally extrapolated figure of 136000 ton/yr blowing on shore

    Modelling the mercury stable isotope distribution of Earth surface reservoirs: Implications for global Hg cycling

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    Mercury (Hg) stable isotopes are useful to understand Hg biogeochemical cycling because physical, chemical and biological processes cause characteristic Hg isotope mass-dependent (MDF) and mass-independent (MIF) fractionation. Here, source Hg isotope signatures and process-based isotope fractionation factors are integrated into a fully coupled, global atmospheric-terrestrial-oceanic box model of MDF (delta Hg-202), odd-MIF (Delta Hg-199) and even-MIF (Delta Hg-200). Using this bottom-up approach, we find that the simulated Hg isotope compositions are inconsistent with the observations. We then fit the Hg isotope enrichment factors for MDF, odd-MIF and even-MIF to observational Hg isotope constraints. The MDF model suggests that atmospheric Hg-0 photo-oxidation should enrich heavy Hg isotopes in the reactant Hg-0, in contrast to the experimental observations of Hg-0 photo-oxidation by Br. The fitted enrichment factor of terrestrial Hg-0 emission in the odd-MIF model (5 parts per thousand) is likely biased high, suggesting that the terrestrial Hg-0 emission flux (160 Mg yr(-1)) used in our standard model is underestimated. In the even-MIF model, we find that a small positive atmospheric Hg-0 photo-oxidation enrichment factor (0.22 parts per thousand) along with enhanced atmospheric Hg-II photo-reduction and atmospheric Hg-0 dry deposition (foliar uptake) fluxes to the terrestrial reservoir are needed to match Delta Hg-200 observations. Marine Hg isotope measurements are needed to further expand the use of Hg isotopes in understanding global Hg cycling. (C) 2018 Elsevier Ltd. All rights reserved

    Climatic Controls on a Holocene Mercury Stable Isotope Sediment Record of Lake Titicaca

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    Mercury (Hg) records in sediment archives inform past patterns of Hg deposition and the anthropogenic contribution to global Hg cycling. Natural climate variations complicate the interpretation of past Hg accumulation rates (HgARs), warranting additional research. Here, we investigated Hg stable isotopes in a ca. 8k year-long sediment core of Lake Titicaca and combined isotopic data with organic biomarkers and biogeochemical measurements. A wet period in the early Holocene (8000-7300 BP) induced strong watershed erosion, leading to a high HgAR (20.2 ± 6.9 μg m -2 year -1 ), which exceeded the 20th century HgAR (8.4 ± 1.0 μg m -2 year -1 ). Geogenic Hg input dominated during the early Holocene ( f geog = 79%) and played a minor role during the mid- to late Holocene (4500 BP to present; f geog = 20%) when atmospheric Hg deposition dominated. Sediment Δ 200 Hg values and the absence of terrestrial lignin biomarkers suggest that direct lake uptake of atmospheric Hg(0), and subsequent algal scavenging of lake Hg, represented an important atmospheric deposition pathway (42%) during the mid- to late Holocene. During wet episodes of the late Holocene (2400 BP to present), atmospheric Hg(II) deposition was the dominant source of lake sediment Hg (up to 82%). Sediment Δ 199 Hg values suggest that photochemical reduction and re-emission of Hg(0) occurred from the lake surface. Hg stable isotopes show promise as proxies for understanding the history of Hg sources and transformations and help to disentangle anthropogenic and climate factors influencing HgAR observed in sediment archives

    Timing and Provenance of Volcanic Fluxes Around the Permian‐Triassic Boundary Mass Extinction in South China: U‐Pb Zircon Geochronology, Volcanic Ash Geochemistry and Mercury Isotopes

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    Anomalous mercury (Hg) contents recorded near the Permian‐Triassic boundary (PTB) are often linked to Siberian Traps Large Igneous Province (STLIP) volcanism and the Permian‐Triassic boundary mass extinction (PTBME). However, mounting evidence indicates that the relation between STLIP volcanism and Hg “anomalies” is not straightforward. This study focuses on the timing and provenance of volcanic fluxes around the PTBME in South China. We constrain carbon isotope (δ13^{13}C) and Hg concentration and isotope records by utilizing high‐precision U‐Pb zircon ages from two expanded deep‐water marine sections spanning the Late Permian to Early Triassic in the Nanpanjiang Basin. Results reveal two episodes of Hg enrichment. The oldest episode predates the onset of a large negative δ13^{13}C excursion, which is documented to be older than 252.07 ± 0.130 Ma. The second episode occurred between 251.822 ± 0.060 and 251.589 ± 0.062 Ma, coinciding with the nadir of the δ13^{13}C excursion. Volcanic ash geochemistry and Hg isotope compositions suggest that mercury was mainly sourced from subduction‐related volcanic arc magmatism in the Tethys region, which peaked between 251.668 ± 0.079 and 251.589 ± 0.052 Ma. These results are compatible with suggestions that regional arc volcanism contributed to the causes of the PTBME in South China and provide evidence that Hg anomalies close to the PTB are not a reliable stratigraphic marker for the PTB extinction event. This study demonstrates that relations between volcanism, environmental perturbations and mass extinction during the Permian‐Triassic transition are better resolved with the aid of high‐precision U‐Pb zircon ages

    Holocene Atmospheric Mercury Levels Reconstructed from Peat Bog Mercury Stable Isotopes

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    Environmental regulations on mercury (Hg)emissions and associated ecosystem restoration are closely linked to what Hg levels we consider natural. It is widely accepted that atmospheric Hg deposition has increased by a factor 3 ± 1 since preindustrial times. However, no long-term historical records of actual atmospheric gaseous elemental Hg (GEM) concentrations exist. In this study we report Hg stable isotope signatures in Pyrenean peat records (southwestern Europe) that are used as tracers of Hg deposition pathway (Δ200Hg, wet vs dry Hg deposition) and atmospheric Hg sources and cycling (δ202Hg, Δ199Hg). By anchoring peatderived GEM dry deposition to modern atmospheric GEM levels we are able to reconstruct the first millennial-scale atmospheric GEM concentration record. Reconstructed GEM levels from 1970 to 2010 agree with monitoring data, and maximum 20th century GEM levels of 3.9 ± 0.5 ng m−3 were 15 ± 4 times the natural Holocene background of 0.27 ± 0.11 ng m−3. We suggest that a −0.7‰ shift in δ202Hg during the medieval and Renaissance periods is caused by deforestation and associated biomass burning Hg emissions. Our findings suggest therefore that human impacts on the global mercury cycle are subtler and substantially larger than currently thought

    Atmospheric Mercury Transfer to Peat Bogs Dominated by Gaseous Elemental Mercury Dry Deposition

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    Gaseous elemental mercury (GEM) is the dominant form of mercury in the atmosphere. Its conversion into oxidized gaseous and particulate forms is thought to drive atmospheric mercury wet deposition to terrestrial and aquatic ecosystems, where it can be subsequently transformed into toxic methylmercury. The contribution of mercury dry deposition is however largely unconstrained. Here we examine mercury mass balance and mercury stable isotope composition in a peat bog ecosystem. We find that isotope signatures of living sphagnum moss (Δ199Hg = −0.11 ± 0.09‰, Δ200Hg = 0.03 ± 0.02‰, 1σ) and recently accumulated peat (Δ199Hg = −0.22 ± 0.06‰, Δ200Hg = 0.00 ± 0.04‰, 1σ) are characteristic of GEM (Δ199Hg = −0.17 ± 0.07‰, Δ200Hg = −0.05 ± 0.02‰, 1σ), and differs from wet deposition (Δ199Hg = 0.73 ± 0.15‰, Δ200Hg = 0.21 ± 0.04‰, 1σ). Sphagnum covered during three years by transparent and opaque surfaces, which eliminate wet deposition, continue to accumulate Hg. Sphagnum Hg isotope signatures indicate accumulation to take place by GEM dry deposition, and indicate little photochemical re-emission. We estimate that atmospheric mercury deposition to the peat bog surface is dominated by GEM dry deposition (79%) rather than wet deposition (21%). Consequently, peat deposits are potential records of past atmospheric GEM concentrations and isotopic composition
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