Terrestrial ecosystems store large amounts of mercury (Hg), which may be subject to methylation, mobilization and uptake into downstream aquatic ecosystems. Mercury concentrations, methylation and ...demethylation potentials are not well characterized simultaneously across different habitats in boreal forest ecosystems, particularly not so in stream sediment, leading to uncertainties about the importance of various habitats as primary production areas of the bioaccumulative neurotoxin methylmercury (MeHg). In this study, we collected soil and sediment samples from 17 undisturbed, central Canadian boreal forested watersheds during spring, summer and fall to robustly characterize the spatial (upland and riparian/wetland soils, and stream sediment) and seasonal patterns of total Hg (THg) and MeHg concentrations. Mercury methylation and MeHg demethylation potentials (Kmeth and Kdemeth) in the soils and sediment were also assessed using enriched stable Hg isotope assays. We found the highest Kmeth and %-MeHg in stream sediment. In both riparian and wetland soils, Hg methylation was lower and less seasonally variable compared to stream sediment, but had comparable MeHg concentrations, suggesting longer-term storage of MeHg produced in these soils. Soil and sediment carbon content, and THg and MeHg concentrations were strong covariates across habitats. Additionally, sediment carbon content was important for delineating between stream sediment with relatively high vs. relatively low Hg methylation potential, which generally separated between different landscape physiographies. Broadly, this large and spatiotemporally diverse dataset is an important baseline for understanding Hg biogeochemistry in boreal forests both in Canada and possibly in many other boreal systems globally. This work is particularly important with respect to future possible impacts from natural and anthropogenic perturbations, which are increasingly straining boreal ecosystems in various parts of the world.
Display omitted
•Measured mercury levels and methylation/demethylation potentials in boreal soils and sediment•Methylmercury production was greatest in stream sediment.•Riparian and wetland soils appear to store methylmercury longer, but produce it more slowly.•Upland soils had low methylmercury content and negligible methylation potentials.•Soil/sediment carbon content, and THg and MeHg concentrations were strong covariates across habitats.
Tracing emission sources and transformations of atmospheric mercury with Hg stable isotopes depends on the ability to collect amounts sufficient for reliable quantification. Commonly employed active ...sampling methods require power and long pumping times, which limits the ability to deploy in remote locations and at high spatial resolution and can lead to compromised traps. In order to overcome these limitations, we conducted field and laboratory experiments to assess the preservation of isotopic composition during sampling of gaseous elemental mercury (GEM) with a passive air sampler (PAS) that uses a sulfur-impregnated carbon sorbent and a diffusive barrier. Whereas no mass independent fractionation (MIF) was observed during sampling, the mass dependent fractionation (MDF, δ
Hg) of GEM taken up by the PAS was lower than that of actively pumped samples by 1.14 ± 0.24‰ (2SD). Because the MDF offset was consistent across field studies and laboratory experiments conducted at 5, 20, and 30 °C, the PAS can be used for reliable isotopic characterization of GEM (±0.3‰ for MDF, ±0.05‰ for MIF, 2SD). The MDF offset occurred more during the sorption of GEM rather than during diffusion. PAS field deployments confirm the ability to record differences in the isotopic composition of GEM (i) with distance from point sources and (ii) sampled at different background locations globally.
Methylmercury (MeHg) is a bioaccumulative neurotoxin produced by certain sulfate-reducing bacteria and other anaerobic microorganisms. Because microorganisms differ in their capacity to methylate ...mercury, the abundance and distribution of methylating populations may determine MeHg production in the environment. We compared rates of MeHg production and the distribution of
genes in epilimnetic sediments from a freshwater lake that were experimentally amended with sulfate levels from 7 to 300 mg L
. The most abundant
sequences were associated with clades of
, sulfate-reducing
,
, and unknown environmental sequences. The
communities from higher sulfate amendments were less diverse and had relatively more
, whereas the communities from lower amendments were more diverse with a larger proportion of
sequences affiliated with other clades. Potential methylation rate constants varied 52-fold across the experiment. Both potential methylation rate constants and % MeHg were the highest in sediments from the lowest sulfate amendments, which had the most diverse
communities and relatively fewer
genes from clades associated with sulfate reduction. Although pore water sulfide concentration covaried with
diversity across our experimental sulfate gradient, major changes in the community of
organisms occurred prior to a significant buildup of sulfide in pore waters. Our results indicate that methylating communities dominated by diverse anaerobic microorganisms that do not reduce sulfate can produce MeHg as effectively as communities dominated by sulfate-reducing populations.
The environmental cycling of mercury (Hg) can be affected by natural and anthropogenic perturbations. Of particular concern is how these disruptions increase mobilization of Hg from sites and alter ...the formation of monomethylmercury (MeHg), a bioaccumulative form of Hg for humans and wildlife. The scientific community has made significant advances in recent years in understanding the processes contributing to the risk of MeHg in the environment. The objective of this paper is to synthesize the scientific understanding of how Hg cycling in the aquatic environment is influenced by landscape perturbations at the local scale, perturbations that include watershed loadings, deforestation, reservoir and wetland creation, rice production, urbanization, mining and industrial point source pollution, and remediation. We focus on the major challenges associated with each type of alteration, as well as management opportunities that could lessen both MeHg levels in biota and exposure to humans. For example, our understanding of approximate response times to changes in Hg inputs from various sources or landscape alterations could lead to policies that prioritize the avoidance of certain activities in the most vulnerable systems and sequestration of Hg in deep soil and sediment pools. The remediation of Hg pollution from historical mining and other industries is shifting towards in situ technologies that could be less disruptive and less costly than conventional approaches. Contemporary artisanal gold mining has well-documented impacts with respect to Hg; however, significant social and political challenges remain in implementing effective policies to minimize Hg use. Much remains to be learned as we strive towards the meaningful application of our understanding for stakeholders, including communities living near Hg-polluted sites, environmental policy makers, and scientists and engineers tasked with developing watershed management solutions. Site-specific assessments of MeHg exposure risk will require new methods to predict the impacts of anthropogenic perturbations and an understanding of the complexity of Hg cycling at the local scale.
•Gaseous elemental mercury (GEM) inhalation remains an occupational exposure concern.•New personal passive sampler has low detection limit, high precision and accuracy.•Mercury is quantified using a ...total mercury analyzer.•A limit of quantification below 25 ng/m3 is achievable over 8-hour deployments.•Sampler is suitable across a range of regulatory thresholds for GEM concentrations.
Inhalation of gaseous elemental mercury (GEM) is an occupational exposure concern for workers handling elemental mercury or mercury-containing waste. GEM is also often present near historically mercury-contaminated sites, potentially resulting in low-level, chronic exposure of the wider population. Here we introduce a passive sampler for personal GEM monitoring which combines a radial porous diffusive barrier with an activated carbon sorbent. A total mercury analyzer is used to quantify GEM sorbed to the carbon by thermal decomposition, amalgamation, and atomic absorption spectroscopy. A sampling rate of 0.070 m3/day was determined by calibrating the sampler at low and high concentrations. Deployments lasting 8 h result in limits of quantification well below 200 ng/m3. The sampler has a measurement range of at least four orders of magnitude. Derived air concentrations were not statistically significantly different from those obtained by active air sampling but were more precise than those obtained using a personal pump. If properly stored, the sampler maintains low blank levels in high GEM environments. Affordability, sturdiness, simplicity, and the wide availability of total mercury analyzers make this sampler highly suited for monitoring GEM inhalation exposure, including in developing countries.
Many wetlands are sources of methylmercury (MeHg) to surface waters, yet little information exists about the distribution of MeHg within wetlands. Total mercury (THg) and MeHg in peat pore waters ...were studied in four peatlands in spring, summer, and fall 2005. Marked spatial variability in the distribution of MeHg, and %MeHg as a proxy for net MeHg production, was observed, with highest values occurring in discrete zones. We denote these zones "MeHg hot spots", defined as an area where the pore water %MeHg exceeded the 90th percentile of the data set (n=463) or >22% of THg as MeHg. MeHg hot spots occurred near the interface between peatland and the upland watershed with few exceptions. The %MeHg in pore water was significantly less in peatland interiors compared to upland-peatland interface zones, with the significance of these differences related to the delineation of the boundary between the two areas. Although further research is necessary, our data suggest that the occurrence of MeHg hot spots is related to the transport of solutes in upland runoff to the peatland perimeter and not to the accumulation of MeHg in this zone as a result of transport from either the peatland interior or the surrounding upland watershed. These findings augment the understanding of peatland MeHg production in upland-peatland watersheds, provide guidance for more accurate quantification of MeHg pool sizes in the landscape, and a spatial framework forthe further study of mercury methylation processes in peatlands.
Methylmercury (MeHg) is the most neurotoxic and bioaccumulative form of mercury (Hg) present in the terrestrial and aquatic food sources of boreal ecosystems, posing potential risks to wildlife and ...human health. Harvesting impacts on Hg methylation and MeHg concentrations in forest soils and stream sediment are not fully understood. In this study, a field investigation was carried out in 4 harvested and 2 unharvested boreal forest watersheds, before and after harvest, to better understand impacts on Hg methylation and MeHg concentration in soils and stream sediment, including their responses to different forest management practices. Changes in total Hg (THg) and MeHg concentrations, first-order potential rate constants for Hg methylation and MeHg demethylation (K
and K
) as well as total carbon content and carbon-to-nitrogen ratio post-harvest in upland, wetland and riparian soils and stream sediment were assessed and compared. Increases in MeHg production were minimal in upland, wetland or riparian soils after harvest. Sediment in streams with minor buffer protection (∼3 m), greater fractions (>75%) of harvested watershed area and more road construction had significantly increased THg and MeHg concentrations, %-MeHg, K
and total carbon content post-harvest. From these patterns, we infer that inputs of carbon and inorganic Hg into harvest-impacted stream sediment are likely sourced from the harvested upland areas and stimulate in situ MeHg production in stream sediment. These findings indicate the importance of stream sediment as potential MeHg pools in harvested forest watersheds. The findings also demonstrate that forest management practices aiming to mitigate organic matter and Hg inputs to streams can effectively alleviate harvesting impacts on Hg methylation and MeHg concentrations in stream sediment.
Methylmercury (MeHg) is a bioaccumulative neurotoxin that is produced by certain anaerobic microorganisms, but the abundance and importance of different methylating populations in the environment is ...not well understood. We combined mercury geochemistry, hgcA gene cloning, rRNA methods, and metagenomics to compare microbial communities associated with MeHg production in two sulfate-impacted lakes on Minnesota's Mesabi Iron Range. The two lakes represent regional endmembers among sulfate-impacted sites in terms of their dissolved sulfide concentrations and MeHg production potential. rRNA amplicon sequencing indicates that sediments and anoxic bottom waters from both lakes contained diverse communities with multiple clades of sulfate reducing Deltaproteobacteria and Clostridia. In hgcA gene clone libraries, however, hgcA sequences were from taxa associated with methanogenesis and iron reduction in addition to sulfate reduction, and the most abundant clones were from unknown groups. We therefore applied metagenomics to identify the unknown populations in the lakes with the capability to methylate mercury, and reconstructed 27 genomic bins with hgcA. Some of the most abundant potential methylating populations were from phyla that are not typically associated with MeHg production, including a relative of the Aminicenantes (formerly candidate phylum OP8) and members of the Kiritimatiellaeota (PVC superphylum) and Spirochaetes that, together, were more than 50% of the potential methylators in some samples. These populations do not have genes for sulfate reduction, and likely degrade organic compounds by fermentation or other anaerobic processes. Our results indicate that previously unrecognized populations with hgcAB are abundant and may be important for MeHg production in some freshwater ecosystems.
Inflammation exerts multiple effects on the early hematopoietic compartment. Best studied is the role of proinflammatory cytokines in activating adult hematopoietic stem and progenitor cells to ...dynamically replenish myeloid lineage cells in a process known as emergency myelopoiesis. However, it is increasingly appreciated that the same proinflammatory signaling pathways are used in diverse hematopoietic scenarios. This review focuses on inflammatory signaling in the emergence of the definitive hematopoietic compartment during embryonic life, and tonic inflammatory signals derived from commensal microbiota in shaping the adult hematopoietic compartment in the absence of pathogenic insults. Insights into the unique and shared aspects of inflammatory signaling that regulate hematopoietic stem and progenitor cell function across the lifespan and health span of an individual will enable better diagnostic and therapeutic approaches to hematopoietic dysregulation and malignancies.
While benzotriazoles (BTs) are ubiquitous in urban waters, their sources and transport remain poorly characterized. We aimed to elucidate the origin and hydrological pathways of BTs in Toronto, ...Canada, by quantifying three BTs, electrical conductivity, and δ
O in high-frequency streamwater samples taken during two rainfall and one snowmelt event in two watersheds with contrasting levels of urbanization. Average concentrations of total BTs (∑BT) were 1.3 to 110 times higher in the more urbanized Mimico Creek watershed relative to the primarily agricultural and suburban Little Rouge Creek. Strong correlations between upstream density of major roads and total BT concentrations or BT composition within all events implicate vehicle fluids as the key source of BTs in both watersheds. Sustained historical releases of BTs within the Mimico Creek watershed have likely led to elevated ∑BT in groundwater, with elevated concentrations observed during baseflow that are diluted by rainfall and surface runoff. In contrast, relatively constant concentrations, caused by mixing of equally contaminated baseflow and rainfall/surface runoff, are observed in the Little Rouge Creek throughout storm hydrographs, with an occasional first flush occurring at a subsite draining suburban land. During snowmelt, buildup of BTs in roadside snowpiles and preferential partitioning of BTs to the liquid phase of a melting snowpack leads to early peaks in ∑BT in both streams, except the sites in the Little Rouge Creek with low levels of vehicle traffic. Overall, a history of BT release and land use associated with urbanization have led to higher levels of BTs in urban areas and provide a glimpse into future BT dynamics in mixed use, (sub)urbanizing areas.
PDF
