Transport Of Hg Research Articles

Underestimated Sink of Atmospheric Mercury in a Deglaciated Forest Chronosequence.

Mercury (Hg) deposition through litterfall has been regarded as the main input of gaseous elemental mercury (Hg0) into forest ecosystems. We hypothesize that earlier studies largely underestimated this sink because the contribution of Hg0 uptake by moss and the downward transport to wood and throughfall is overlooked. To test the hypothesis, we investigated the Hg fluxes contributed via litterfall and throughfall, Hg pool sizes in moss covers and woody biomass as well as their isotopic signatures in a glacier-to-forest succession ecosystem of the Southeast Tibetan Plateau. Results show that Hg0 depositional uptake and pool sizes stored in moss and woody biomass increase rapidly with the time after glacier retreat. Using the flux data as input to a Hg isotopic mixing model, Hg deposition through litterfall accounts for 27-85% of the total accumulation rate of Hg0 in organic soils of glacial retreat over 20-90 years, revealing the presence of additional sources of Hg0 input. Atmospheric Hg0 accounts for 76 ± 24% in ground moss, 86 ± 15% in tree moss, 62-92% in above ground woody biomass (branch-bark-stem), and 44-83% in roots. The downward decreasing gradient of atmospheric Hg0 fractions from the above ground woody biomass to roots suggests a foliage-to-root Hg transport in vegetation after uptake. Additionally, 34-82% of atmospheric Hg0 in throughfall further amplifies the accumulation of Hg0 from atmospheric sources. We conclude that woody biomass, moss, and throughfall represent important Hg0 sinks in forest ecosystems. These previously unaccounted for sink terms significantly increase the previously estimated atmospheric Hg0 sink via litterfall.

The Role of a Tidal Flat–Saltmarsh System as a Source–Sink of Mercury in a Contaminated Coastal Lagoon Environment (Northern Adriatic Sea)

The Marano and Grado Lagoon (northern Adriatic Sea, Italy) is contaminated mainly by mercury (Hg) of mining and industrial origin. This work aims to investigate the sedimentary records of Hg of a tidal flat–saltmarsh (TF–S) system and to understand the role played by tidal fluxes in terms of the transport, accumulation and release of Hg due to the periodic flow of the tide. The complex history of the sources of Hg in the area of the TF–S system has resulted in several fluctuations of Hg in sediments over time; due to its higher sedimentation rate (1.3 cm year−1) than the subtidal areas of the Grado lagoon, the outer area of the TF–S system is more active in terms of accumulation (from 56 to 81 mg m−2 year−1) than the inner area. Fluxes were estimated at the mouth of a principal tidal creek by combining discrete hourly tidal flow measurements with weighed measurements of dissolved (DHg) and particulate (PHg) mercury obtained via water sample collection. Mercury, mainly in particulate form, is drained by the tidal creek from the marsh during a tidal semi-cycle. The highest flux of PHg was recorded during ebb tide in July (1071 mg). The calculation of the quantitative flows of PHg and DHg highlighted a tendency for Hg to be exported from the TF–S to the lagoon channel during a tidal semi-cycle. However, the results obtained here for the Hg fluxes do not allow for the depiction of a constant positive or negative budget as that found in the literature for macro-scale budget calculations at lagoon tidal inlets. A possible explanation for there being no constant trend in the PHg and DHg budget is that our TF–S system is located in a lagoon area where previous findings reported accretion or a balance situation between erosion and sedimentation processes.

Decoupling Natural and Anthropogenic Mercury and Lead Transport from South Asia to the Himalayas.

Mercury (Hg) and lead (Pb) accumulation since the Industrial Revolution has been generally observed to increase concurrently in lake sedimentary records around the world. Located downwind during the monsoon season from the rapidly developing South Asia, the Himalayas and the Tibetan Plateau are expected to receive direct anthropogenic Hg and Pb loadings, yet the source, pathway, and effects of such transport remain poorly known due to logistic challenges in accessing this region. When studying the sediment record from Lake Gokyo (4750 m above sea level (a.s.l.)) in the Himalayas, we find remarkably different Hg and Pb accumulation trends over the past 260 years. Although Hg accumulation has continued to increase since the Industrial Revolution, Pb accumulation peaked during that time and has been decreasing since then. Stable isotope analysis reveals that the decoupling trends between these two elements are due to different sources and pathways of Hg and Pb in the region. Both δ202Hg and Δ199Hg have been increasing since the Industrial Revolution, suggesting that anthropogenic Hg emissions from South Asia have been continuously increasing and that the Indian monsoon-driven wet deposition of atmospheric Hg is the dominant pathway for Hg accumulation in the sediments. In contrast, analysis of 206Pb/207Pb and 208Pb/207Pb ratios suggests that Pb accumulation in the sediments originates primarily from natural sources and that the decreasing trend of Pb accumulation is most likely due to a weakening input of atmospheric mineral dust by the westerlies. These decoupling trends highlight the ongoing issue of transboundary Hg transport to the Himalayas and the Tibetan Plateau that are source waters for major freshwater systems in Asia and calls for regional and international collaborations on Hg emission controls in South Asia.

Mercury Isotope Fractionation during the Photochemical Reduction of Hg(II) Coordinated with Organic Ligands.

The photochemical reduction of Hg(II) is an important pathway in the environmental Hg cycle because it competes with Hg methylation and potentially limits the formation of bioaccumulative methylmercury. Hg stable isotope systematics have proven to be an effective tool for investigating the transport, transformation, and bioaccumulation of Hg. The dominant cause of mass independent isotope fractionation (MIF) of Hg in nature is the photochemical reduction of various species of Hg(II). However, it is difficult to fully interpret Hg stable isotope signatures due to the lack of mechanistic information about which Hg compounds are susceptible to MIF and why. This study investigates Hg isotope fractionation during the photochemical reduction of Hg(II) complexed to organic ligands, which are representative of the available binding sites in natural dissolved organic matter. The photochemical reduction of Hg(II) in the presence of cysteine resulted in both negative and positive MIF in residual Hg(II), where the sign depended on pH and dissolved oxygen level. In the presence of serine, either nuclear volume or magnetic isotope effects were observed depending on the wavelength of light and the extent of Hg(II) complexation by serine. In the presence of ethylenediamine, MIF was negative. Our Hg stable isotope results suggest that MDF and MIF are induced at different steps in the overall photochemical reduction reaction and that MIF does not depend on the rate-determining step but instead depends on photophysical aspects of the reaction such as intersystem crossing and hyperfine coupling. The behavior of Hg isotopes reported here will allow for a better understanding of the underlying reaction mechanisms controlling the Hg isotope signatures recorded in natural samples.

Diffuse emission and transport of gaseous elemental mercury (GEM) in the Mapamyum geothermal system, Western Tibet (China)

Mercury (Hg) is a widely spread pollutant, owing to its high mobility in the nature. The rising input of Hg into the atmosphere has resulted in enhanced Hg pollution in both terrestrial and aquatic ecosystems. The Tibetan plateau, which is known as the roof of the world, is considered as a Hg-sensitive ecosystem. The Himalayan-Tibetan geothermal belt, which is formed due to the collision between India and Eurasia, is an important potential source of Hg to the atmosphere. However, previous studies to the emission and transport of geological Hg in the Tibetan Plateau are still rare. Understanding emission and transport of Hg in the Tibetan Plateau can provide important constraints on global Hg budget and its pollution transport. Diffuse emission and transport of gaseous elemental mercury (GEM or Hg0) in the Mapamyum geothermal system (MGF) of western Tibet was investigated and simulated by the closed-chamber method and the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) dispersion model. The estimated annual output of GEM in the MGF, calculated over an area of 41,615 m2, was in the order of 6.1 × 10−4 ton. He-C isotope ratios of the geothermal samples were all within the range of typical crustal domain. Combing with the hydrothermal analysis, it could deduce the Hg0 in the MGF might derive from both deep lithosphere and the upper crust. The GEM diffused from the source region was mainly dispersed to the NW direction. The maximum concentration of GEM is mainly distributed around the MGF, which is also the region with the largest deposition rate. The simulated results of the HYSPLIT dispersion model suggest that the GEM emitted from the MGF would not significantly enhance the atmospheric Hg concentration, whereas the deposition and accumulation of GEM around the source region is not negligible.

Mercury transport and fate in municipal solid waste landfills and its implications

Mercury (Hg) release and migration from municipal solid waste landfills has been an important issue to nearby ecosystems and human health. To completely understand the Hg biogeochemical cycle in landfills, this review presents the Hg emission processes via different pathways, related controlling mechanisms, and critical Hg transport and transformation processes involving the diffusion and advection of Hg, Hg volatilization, Hg adsorption and desorption, Hg redox reactions, and Hg methylation and demethylation. These critical physical, chemical, and biological processes result in the phase transfer of Hg and the distribution of different Hg species in landfill gas (LFG), leachates, and cover soils. In addition, key factors (e.g., LFG, meteorological conditions, cover soils, and vegetation) affecting Hg emission processes and their impacts are discussed here. This work provides a comprehensive picture of Hg behavior in landfills, and has positive implications for the development of a process-based model and the control of Hg emissions from landfills.

Elemental mercury in the marine boundary layer of North America: Temporal and spatial patterns

Gaseous elemental mercury (Hg0) comprises the majority of atmospheric mercury (Hg) and results in long-range transport of Hg. Secondary emissions from the marine surface mixed layer result in spatial and temporal Hg0 variability, which subsequently determine marine pools of divalent mercury (HgII) available for methylation. We measured atmospheric Hg0 concentrations in the marine boundary layer (MBL) around North America in regions of the Atlantic, Pacific, and Arctic Oceans (6.7°–77.3° N, 52.3°–150.0° W). Observed spatial Hg0 distributions across these regions match patterns revealed from current published biogeochemical models. These models have supported marine processes as the major factors controlling MBL Hg0. We observe differences in variability between ocean basins. Asian emissions appear to be well-mixed in the Eastern Pacific MBL, with stable measurements across a 3200 km transect in the North Pacific. Hg0 concentrations decrease but remain relatively stable in tropical regions of the Pacific and Atlantic. In contrast, we measured several 100–200 km regions of elevated Hg0 above North Atlantic surface waters. Repeated offshore sampling of Arctic Hg0 reveals strong seasonal trends that are similar to those collected at coastal long-term Arctic monitoring stations. These similarities suggest marine processes control seasonal Arctic trends, which are linked to sea ice formation and melt. Together our observations are consistent with marine controls on MBL Hg0 concentrations although further study is needed to fully distinguish between marine and atmospheric controls.

Probing the Role of the Chloroplasts in Heavy Metal Tolerance and Accumulation in Euglena gracilis.

The E. gracilis Zm-strain lacking chloroplasts, characterized in this study, was compared with the earlier assessed wild type Z-strain to explore the role of chloroplasts in heavy metal accumulation and tolerance. Comparison of the minimum inhibitory concentration (MIC) values indicated that both strains tolerated similar concentrations of mercury (Hg) and lead (Pb), but cadmium (Cd) tolerance of the Z-strain was twice that of the Zm-strain. The ability of the Zm-strain to accumulate Hg was higher compared to the Z-strain, indicating the existence of a Hg transportation and accumulation mechanism not depending on the presence of chloroplasts. Transmission electron microscopy (TEM) showed maximum accumulation of Hg in the cytosol of the Zm-strain and highest accumulation of Cd in the chloroplasts of the Z-strain indicating a difference in the ability of the two strains to deposit heavy metals in the cell. The highly abundant heavy metal transporter MTP2 in the Z-strain may have a role in Cd transportation to the chloroplasts. A multidrug resistance-associated protein highly increased in abundance in the Zm-strain could be a potential Hg transporter to either cytosol or mitochondria. Overall, the chloroplasts appear to have major role in the tolerance and accumulation of Cd in E. gracilis.

Near-Decadal Oscillation of Water Levels and Mercury Bioaccumulation in the Laurentian Great Lakes Region

Mercury (Hg) contamination in remote lakes stems from atmospheric Hg transport to surface waters and subsequent conversion by microbes to neurotoxic methylmercury (MeHg) that biomagnifies in pelagi...

Total mercury and methylmercury migration and transformation in an A2/O wastewater treatment plant

Municipal wastewater treatment plants (MWTPs) serve an essential role in reducing mercury (Hg) pollution. However, few studies quantified the transport and transformation of Hg through MWTPs, particularly plants based on the anaerobic-anoxic-aerobic (A2/O) process. Here, we present a mass balance for total mercury (THg) and total methylmercury (TMeHg) at the plant, and investigate the influence of pH, temperature, and dissolved oxygen on the occurrence and fate of methylmercury (MeHg) in the system. The concentrations of the THg and TMeHg in the raw sewage were 40.3 ± 26.6 ng/L (4.3 ± 2.7 g/day) and 1.9 ± 0.6 ng/L (193 ± 58 mg/day), respectively. Their concentrations in the plant's effluent water were 7.4 ± 1.5 ng/L (0.74 ± 0.2 g/day) and 0.04 ± 0.01 ng/L (3.9 ± 1.0 mg/day), corresponding to decreases of ~82% for THg and ~98% for TMeHg. Within the plant, only ~10% of the THg was removed with primary sedimentation, as Hg in the raw sewage was predominately in dissolved form. In contrast, a significant portion of TMeHg (~43%) was associated with incoming particulate matter. Much of the remaining Hg was removed in subsequent A2/O process and secondary clarifiers, with a ~78% of the THg entering the plant transferring to the dewatered sludge (concentration 1.05 ± 0.28 μg/g; 3.2 ± 0.8 g/day). These same steps decreased TMeHg in the water by ~95%, with <10% of that reduction being TMeHg transferred to the sludge (concentration 2.1 ± 1.1 ng/g; 6.2 ± 3.3 mg/day), suggesting >90% TMeHg degradation. In addition, the most important factor that impacted the variation of TMeHg concentrations was pH, then was temperature. Dissolved oxygen showed no relationship with TMeHg and DMeHg. Overall, this study demonstrates that A2/O MWTPs effectively remove MeHg from wastewater, however, sludge remains an important potential source of Hg to the environment.

Organic matters and acid‐sulfate alteration in Itomuka mercury mine, Hokkaido, Japan: Implications for the transportation and deposition mechanisms of Hg

AbstractIn order to examine the transportation and deposition mechanisms of Hg, we investigated the ore and hydrothermal alteration minerals and solid organic matters from Itomuka mercury mine located in the eastern part of central Hokkaido. In addition to the ore minerals, native mercury and cinnabar, quartz, marcasite, alunite, kaolinite, and minor amounts of pyrite and smectite were identified in the Hg ore by powder X‐ray diffraction (XRD) analysis. This mineral assemblage of acid sulfate alteration was likely developed under the conditions of low temperature (≤100°C) and low pH (≤2) in the steam‐heated environment. The H2SO4 was produced above the water table by the oxidation of H2S separated from deep, near‐neutral fluids by boiling. The dominance of native mercury over cinnabar in Hg ore indicates that the greater part of mineralized Hg was transported as Hg0 in aqueous solution and vapor with low sulfur fugacity. The solid organic matters found in the Hg ore were analyzed with SEM‐EDS, micro‐XRD, and micro‐Fourier transform infrared (FTIR) spectroscopy, and these results suggest that the organic matters contributed to keeping the low fO2 of the Hg‐bearing fluid and transportation of Hg as Hg0 in S‐poor condition. Because the solubility of Hg in acidic fluid is low, neutral to alkaline fluid seems to have leached Hg from the basement sedimentary rocks of Hidaka Group which also supplied the organic matters to the fluid. The oxidation and cooling of Hg‐bearing solution and vapor triggered the deposition of liquid Hg as a primary phase.

Deforestation Due to Artisanal and Small-Scale Gold Mining Exacerbates Soil and Mercury Mobilization in Madre de Dios, Peru.

Artisanal and small-scale gold mining (ASGM) is a significant contributor of mercury (Hg) contamination and deforestation across the globe. In the Colorado River watershed in Madre de Dios, Peru, mining and deforestation have increased exponentially since the 1980s, resulting in major socioeconomic shifts in the region and two national state of emergency (2016 and 2019) in response to concerns for wide-scale mercury poisoning by these activities. This research employed a watershed-scale soil particle detachment model and environmental field sampling to estimate the role of land cover change and soil erosion on river transport of Hg in a heavily ASGM-impacted watershed. The model estimated that observed decreases in forest cover increased soil mobilization by a factor of two in the Colorado River watershed during the 18 year period and by 4-fold in the Puquiri subwatershed (the area of most concentrated ASGM activity). If deforestation continues to increase at its current exponential rate through 2030, the annual mobilization of soil and Hg may increase by an additional 20-25% relative to 2014 levels. While, the estimated total mass of Hg transported by rivers is substantially less than the estimated tons of Hg used with ASGM in Peru, this research shows that deforestation associated with ASGM is an additional mechanism for mobilizing naturally occurring and anthropogenic Hg from terrestrial landscapes to aquatic environments in the region, potentially leading to bioaccumulation in fish and exposure to communities downstream.

Mercury accumulation in soil from atmospheric deposition in temperate steppe of Inner Mongolia, China

Mercury (Hg) is a toxic and persistent pollutant and has long-term impacts on ecological systems and human health. Coal-fired power plants (CFPPs) are the main source of anthropogenic Hg emission, and the emitted atmospheric Hg is deposited to the surrounding environments which causes soil pollution. To assess the effects of atmospheric Hg from CFPPs in China on the temperate steppe, Hg contents in the topsoil and subsoil were analyzed for samples collected from 80 sites in central Inner Mongolia during 2012–2015. The average content of Hg in topsoil and subsoil were 14.9 ± 10.4 μg kg−1 and 8.9 ± 5.8 μg kg−1, respectively. The principal components analysis (PCA) indicated that the soil organic matter content and atmospheric deposition were the main factors determining soil Hg content in Inner Mongolia. We used the power plant impact factor (PPIF) to evaluate the impacts of the surrounding CFPPs. The PPIF results showed the most positive correlation with Hg content in topsoil at more than 400 km distances, indicating that the contribution of the long-range transport of Hg emitted from CFPPs is regional in scale. Considering the potential of Hg accumulation in soil, long-term and regional measurements of soil Hg and stricter emission-limit standards for power plants should be implemented to control soil Hg pollution in China.

Less metal fluxes than expected from fibrous marine sediments

Deposits of fibrous sediment, which include fiberbanks and fiber-rich sediments, are known to exist on the Swedish seafloor adjacent to coastally located former pulp and paper industries. These deposits contain concentrations of hazardous substances that exceed national background levels and contravene national environmental quality objectives (EQOs). In this study of metal fluxes from fibrous sediments using benthic flux chamber measurements (BFC) in situ we obtained detected fluxes of Co, Mo, Ni and Zn, but no fluxes of Pb, Hg and Cr. The absence of fluxes of some of the analyzed metals indicates particle bound transport of Pb, Cr and Hg from fiberbanks even though Hg might become methylated under anoxic conditions and, in that case, may enter the food chain. We found less metal fluxes than expected and thus emphasize the importance of in-situ flux measurements as a compliment to sediment metal concentrations within risk assessments of contaminated sediments.

Mercury and dissolved organic matter dynamics during snowmelt runoff in a montane watershed, Provo River, Utah, USA

The mechanisms of Hg and dissolved organic matter (DOM) transport from watersheds to streams remain unclear, especially in snowmelt dominated montane systems. We characterized total Hg concentrations and DOM characteristics during snowmelt by weekly and/or monthly sampling at three locations in the upper Provo River, northern Utah, over two water years (2016 and 2017). Total Hg concentrations increased from <1 ng/L during baseflow to >7 ng/L during the snowmelt period (April–June), with decreasing concentrations from upstream to downstream. Filtered THg concentrations accounted for 65–75% of the unfiltered concentrations, suggesting that Hg is primarily transported in the dissolved phase. Annual THg loading in the upper Provo River was approximately 1 kg/yr, with ~90% of the flux occurring during the snowmelt period. Filtered THg concentrations were strongly correlated with in-situ fluorescence DOM (fDOM) measurements, allowing for the development of high-resolution proxy THg concentrations. Further, DOM characteristics, evaluated using excitation-emission matrices (EEMs) and parallel factor analysis (PARAFAC), identified the dominance of soil humic and fulvic acid fractions of DOM during runoff. Total Hg concentrations were low in snowpack but elevated in ephemeral streams during snowmelt runoff, indicating that Hg originated from shallow soil water rather than snow. Concentration—discharge relationships revealed clockwise hysteresis patterns, suggesting that Hg was flushed from soils on the rising limb of the hydrograph. Our results demonstrate that a majority of Hg transport occurs with a flux of DOM during the short snowmelt season as shallow soils are flushed by meltwater. The snowmelt-driven Hg pulse is a substantial source to downstream reservoirs and potentially contributes to a fish consumption advisory.

Comparative study of the effects of different chelating ligands on the absorption and transport of mercury in maize (Zea mays L.)

Mercury (Hg) pollution seriously threatens food safety and has attracted global attention. Phytoextraction, due to its low cost, applicability, and environmental friendliness, is considered a new technology for clean-up of heavy metal contamination in the environment. However, the low bioavailability of Hg in polluted areas greatly limits the applicability of phytoextraction. Here, we compared the effects of six common chelating ligands on the absorption and transport of Hg in maize (Zea mays L.), which has a high biomass and short growth cycle. The results showed that the root length and biomass of maize seedlings of the groups treated with the six chelating ligands (EDTA, iodide, ammonium, thiosulfate, thiocyanate, and thiocarbamide) did not change compared with those of the non-treated groups. Co-exposure to Hg and each chelating ligand markedly alleviated the inhibitory effect induced by Hg. Iodide treatment resulted in the lowest root Hg content and highest translocation factor (TF) value, while ammonium treatment gave rise to the highest shoot Hg concentration and lowest TF. Compared with other chelating ligands, thiosulfate exhibited the maximum alleviation of Hg toxicity and achieved the highest concentration of Hg in the roots and aerial parts. Moreover, the TF and Hg accumulation in the thiosulfate and Hg co-exposed group were much higher than those in the group exposed to Hg alone. This finding suggests that, among these common chelating ligands, thiosulfate compounds have great potential for Hg phytoextraction, while the others can immobilize Hg in polluted areas.

Mercury fluxes, budgets, and pools in forest ecosystems of China: A review

Mercury (Hg) retention in forest ecosystem plays a key role in global biogeochemical cycling. We present a comprehensive review of the research status of forest Hg in China to characterize the Hg budgets and pools. Averaged total Hg (THg) inputs at remote forests and rural and suburban forests in China are about 2–4-fold and 2.5–5-fold higher than the observed values in Europe and North America, respectively. The highly elevated THg inputs are mainly derived from the elevated atmospheric Hg concentrations and litterfall biomass. THg outputs from the forest ecosystems are much lower than the atmospheric depositions. The annual THg retentions range from 26.1 to 60.4 µg m−2 at subtropical forests and from 12.4 to 26.2 µg m−2 at temperate forests. Given the large areal coverage, THg retention in forest is ∼69 t year−1 in China and is much high than that in global scale estimated by models. The much higher THg retention has elevated the THg pools in Chinese subtropical forests. This study has implication for the role of China forests in the global Hg biogeochemical cycle and the optimization of atmospheric Hg transport and deposition models.

Comparison of Mercury Contamination in Four Indonesian Watersheds Affected by Artisanal and Small-Scale Gold Mining of Varying Scale

Artisanal and small-scale gold mining (ASGM) accounts for almost half of anthropogenic mercury (Hg) emissions worldwide and causes widespread water pollution. In Indonesia, several studies have identified harmful levels of Hg in areas affected by ASGM. While most of these studies focus on mining areas with thousands of miners, water contamination in smaller ASGM areas is less understood. We evaluated Hg contamination in four ASGM areas in Central Java of varying scale (from 30 to 3000 amalgamator barrels at each area), including Jatiroto, Kebonsari, Gumelar, and Kulon Progo. At each location, we collected water samples along river transects upstream and downstream of ASGM areas during the dry season (June–July 2017). Total Hg (THg) concentrations in stream water increased by orders of magnitude from upstream to downstream of ASGM activities at Jatiroto (1.35–4730 ng/L), with smaller observed increases at the other locations. Dissolved THg concentrations exceeded USEPA criteria for aquatic life (12 ng/L) at two of the four ASGM areas. THg concentrations in tailings exceeded 150,000 ng/L. Notably, THg concentrations in stream water were not directly related to the scale of mining, with Jatiroto having the highest concentrations as second smallest mining areas of the four in this study. Downstream of the mining areas, the fraction of dissolved methyl Hg to dissolved THg reached 20%, indicating that active Hg methylation occurs in the watersheds. Further study is needed to investigate Hg transport in the wet season when rainfall and high stream discharge may mobilize contaminated sediment near mining areas.

Paleoclimatic controls on mercury deposition in northeast Brazil since the Last Interglacial

The sediment core GL-1248, collected from the continental slope off northeastern Brazil, was used to reconstruct mercury (Hg) variations in NE South American continental margin and understand its variability in response to paleoclimate changes over the past 128 ka. Mercury concentrations in GL-1248 ranged between 14.95 and 69.43 ng/g, showing a glacial-interglacial pattern with higher (lower) concentrations in the glacial period (interglacial period). Parallel trends of Hg and XRF-Fe plots suggest that following atmospheric Hg deposition onto the continent, Hg is incorporated with Fe compounds before transportation and eventual immobilization at the NE Brazil continental slope. Peaks of Hg and Fe/Ca ratio peaks occurred concurrently during certain Heinrich Stadials, indicating that Hg is transported from the continent alongside fluvial sediments during periods of increased precipitation and erosion in NE Brazil continent. Mercury concentrations varied with periodicities of 56 ka and 900 yr suggesting glacial-interglacial changes and millennial-scale variability, respectively. Total Hg and total organic carbon are poorly correlated, although the latter likely influenced Hg sequestration into marine sediments during millennial-scale events between 60 ka and 30 ka. Altogether, our results suggest that the atmosphere is the primary source of Hg to GL-1248 and glacial-interglacial climate variations were the major determinant of atmospheric Hg deposition. Furthermore, increased precipitation during millennial-scale events played a secondary role by enhancing Hg transport to the continental slope of NE Brazil.

Mercury isotopic signatures of tailings from artisanal and small-scale gold mining (ASGM) in southwestern Ecuador

Artisanal and small-scale gold mining (ASGM) is currently one of the largest anthropogenic sources of mercury (Hg) to the atmosphere and a significant source to downstream terrestrial aquatic systems. Given the potential toxicity of Hg when it is released to aquatic ecosystems, both scientific and regulatory communities have interest in the development of tools and methods for understanding the fate and transport of Hg in the environment. Although Hg isotopes are applied extensively to trace other anthropogenic point sources of Hg in aquatic ecosystems, few studies have used isotopic analyses to investigate the downstream impacts of ASGM. Furthermore, these studies are currently limited by relatively sparse Hg isotopic analyses on ASGM materials. In this study, ASGM samples from Portovelo-Zaruma (Ecuador), representing various stages of the processing of low-grade gold-bearing ores, were analyzed for Hg concentrations and stable isotope ratios. These data were used to assess the isotopic variability of the ASGM endmember and confirm the results of prior isotopic analyses of ASGM materials and downstream sediments from Portovelo-Zaruma. While the Hg concentrations of the ASGM samples varied significantly, isotopic analyses revealed a limited range of signatures that was characterized by relatively heavy mass-dependent fractionation (MDF) with little to no significant mass-independent fractionation (MIF). The signatures of ASGM samples analyzed in this study matched well with previously reported ASGM samples from Portovelo-Zaruma as well as downstream sediments (for up to 120 km). Furthermore, the overall Hg isotopic compositions of potential ASGM endmembers are distinct from typical compositions observed in freshwater ecosystems (e.g., from soil erosion, atmospheric deposition), allowing Hg isotopes to be a powerful tool in tracing downstream Hg contamination from ASGM.