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Bumblebees are key pollinators with gut microbiotas that support host health. After bumblebee queens undergo winter diapause, which occurs before spring colony establishment, their gut microbiotas are disturbed, but little is known about community dynamics during diapause itself. Queen gut microbiotas also help seed worker microbiotas, so it is important that they recover post-diapause to a typical community structure, a process that may be impeded by pesticide exposure. We examined how bumblebee queen gut microbiota community structure and metabolic potential shift during and after winter diapause, and whether post-diapause recovery is affected by pesticide exposure. To do so, we placed commercial Bombus impatiens queens into diapause, euthanizing them at 0, 2 and 4 months of diapause. Additionally, we allowed some queens to recover from diapause for 1 week before euthanasia, exposing half to the common herbicide glyphosate. Using whole-community, shotgun metagenomic sequencing, we found that core bee gut phylotypes dominated queen gut microbiotas before, during and after diapause, but that two phylotypes, Schmidhempelia and Snodgrassella, ceased to be detected during late diapause and recovery. Despite fluctuations in taxonomic community structure, metabolic potential remained constant through diapause and recovery. Also, glyphosate exposure did not affect post-diapause microbiota recovery. However, metagenomic assembly quality and our ability to detect microbial taxa and metabolic pathways declined alongside microbial abundance, which was substantially reduced during diapause. Our study offers new insights into how bumblebee queen gut microbiotas change taxonomically and functionally during a key life stage and provides guidance for future microbiota studies in diapausing bumblebees., (© 2024 The Author(s). Insect Molecular Biology published by John Wiley & Sons Ltd on behalf of Royal Entomological Society.)

Social bees are frequently exposed to pesticides when foraging on nectar and pollen. Recent research has shown that pesticide exposure not only impacts social bee host health but can also alter the community structure of social bee gut microbiotas. However, most research on pesticide-bee gut microbiota interactions has been conducted in honey bees; bumble bees, native North American pollinators, have received less attention and, due to differences in their ecology, may be exposed to certain pesticides for shorter durations than honey bees. Here, we examine how exposure to the fungicide chlorothalonil for a short, field-realistic duration alters bumble bee fecal microbiotas (used as a proxy for gut microbiotas) and host performance. We expose small groups of Bombus impatiens workers (microcolonies) to field-realistic chlorothalonil concentrations for 5 days, track changes in fecal microbiotas during the exposure period and a recovery period, and compare microcolony offspring production between treatments at the end of the experiment. We also assess the use of fecal microbiotas as a gut microbiota proxy by comparing community structures of fecal and gut microbiotas. We find that chlorothalonil exposure for a short duration does not alter bumble bee fecal microbiota structure or affect microcolony production at any concentration but that fecal and gut microbiotas differ significantly in community structure. Our results show that, at least when exposure durations are brief and unaccompanied by other stressors, bumble bee microbiotas are resilient to fungicide exposure. Additionally, our work highlights the importance of sampling gut microbiotas directly, when possible.IMPORTANCEWith global pesticide use expected to increase in the coming decades, studies on how pesticides affect the health and performance of animals, including and perhaps especially pollinators, will be crucial to minimize negative environmental impacts of pesticides in agriculture. Here, we find no effect of exposure to chlorothalonil for a short, field-realistic period on bumble bee fecal microbiota community structure or microcolony production regardless of pesticide concentration. Our results can help inform pesticide use practices to minimize negative environmental impacts on the health and fitness of bumble bees, which are key native, commercial pollinators in North America. We also find that concurrently sampled bumble bee fecal and gut microbiotas contain similar microbes but differ from one another in community structure and consequently suggest that using fecal microbiotas as a proxy for gut microbiotas be done cautiously; this result contributes to our understanding of proxy use in gut microbiota research., Competing Interests: The authors declare no conflict of interest.

The production of methylmercury (MeHg) in flooded paddy fields determines its accumulation in rice grains; this, in turn, results in MeHg exposure risks for not only rice-eating humans but also wildlife. Nitrogen (N) fertilizers have been widely applied in rice cultivation fields to supply essential nutrients. However, the effects of N fertilizer addition on mercury (Hg) transformations are not unclear. This limits our understanding of MeHg formation in rice paddy ecosystems. In this study, we spiked three Hg tracers ( 200 Hg II , Me 198 Hg, and 202 Hg 0 ) in paddy slurries fertilized with urea, ammonium, and nitrate. The influences of N fertilization on Hg methylation, demethylation, and reduction and the underlying mechanisms were elucidated. The results revealed that dissimilatory nitrate reduction was the dominant process in the incubated paddy slurries. Nitrate addition inhibited Hg II reduction, Hg II methylation, and MeHg demethylation. Competition between nitrates and other electron acceptors (e.g., Hg II , sulfate, or carbon dioxide) under dark conditions was the mechanism underlying nitrate-regulated Hg transformation. Ammonium and urea additions promoted Hg II reduction, and anaerobic ammonium oxidation coupled with Hg II reduction (Hgammox) was likely the reason. This work highlighted that nitrate addition not only inhibited Hg II methylation but also reduced the demethylation of MeHg and therefore may generate more accumulation of MeHg in the incubated paddy slurries. Findings from this study link the biogeochemical cycling of N and Hg and provide crucial knowledge for assessing Hg risks in intermittently flooded wetland ecosystems., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Methylmercury (MeHg) is a microbially produced neurotoxin derived from inorganic mercury (Hg), which accumulation in rice represents a major health concern to humans. However, the microbial control of MeHg dynamics in the environment remains elusive. Here, leveraging three rice paddy fields with distinct concentrations of Hg (Total Hg (THg): 0.21-513 mg kg -1 dry wt. soil; MeHg: 1.21-6.82 ng g -1 dry wt. soil), we resorted to metagenomics to determine the microbial determinants involved in MeHg production under contrasted contamination settings. We show that Hg methylating Archaea, along with methane-cycling genes, were enriched in severely contaminated paddy soils. Metagenome-resolved Genomes of novel putative Hg methylators belonging to Nitrospinota (UBA7883), with poorly resolved taxonomy despite high completeness, showed evidence of facultative anaerobic metabolism and adaptations to fluctuating redox potential. Furthermore, we found evidence of environmental filtering effects that influenced the phylogenies of not only hgcA genes under different THg concentrations, but also of two housekeeping genes, rpoB and glnA, highlighting the need for further experimental validation of whether THg drives the evolution of hgcAB. Finally, assessment of the genomic environment surrounding hgcAB suggests that this gene pair may be regulated by an archaeal toxin-antitoxin (TA) system, instead of the more frequently found arsR-like genes in bacterial methylators. This suggests the presence of distinct hgcAB regulation systems in bacteria and archaea. Our results support the emerging role of Archaea in MeHg cycling under mining-impacted environments and shed light on the differential control of the expression of genes involved in MeHg formation between Archaea and Bacteria., (© 2023. The Author(s).)

Mine tailings are prevalent worldwide and can adversely impact adjacent ecosystems, including wetlands. This study investigated the impact of gold (Au) mine tailings contamination on peatland soil and pore water geochemistry, vegetation and microbial communities, and microbial carbon (C) cycling. Maximum arsenic (As) concentrations in peat and pore water reached 20,137 mg kg -1 and 16,730 μg L -1 , respectively, but decreased by two orders of magnitude along a 128 m gradient extending from the tailings into the wetland. Carbon and other macronutrient (N, P, K) concentrations in peat and pore water significantly increased with distance from contamination. Relative percent cover and species richness of vascular and non-vascular plants significantly increased with distance into the wetland, with higher non-vascular richness being found at intermediate distances before transitioning to a vascular plant dominated community. Bacterial and archaeal community composition exhibited a decreased proportion of members of the phylum Acidobacteria (notably of the order Acidobacteriales) and increased diversity and richness of methanogens across a larger range of orders farther from the tailings source, an indication of microbial C-cycling potential. Consistent with changes in microbial communities, in vitro microbial CH 4 production potential significantly increased with distance from the contaminant source. This study demonstrates both the profound negative impact that metalliferous tailings contamination can have on above and belowground communities in peatlands, and the value of wetland preservation and restoration., Competing Interests: Declaration of competing interest Editorial Board of Science of the Total Environment - Shaun Watmough, (Copyright © 2023 Elsevier B.V. All rights reserved.)

Methylmercury (MeHg) contamination in rice via paddy soils is an emerging global environmental issue. An understanding of mercury (Hg) transformation processes in paddy soils is urgently needed in order to control Hg contamination of human food and related health impacts. Sulfur (S)-regulated Hg transformation is one important process that controls Hg cycling in agricultural fields. In this study, Hg transformation processes, such as methylation, demethylation, oxidation, and reduction, and their responses to S input (sulfate and thiosulfate) in paddy soils with a Hg contamination gradient were elucidated simultaneously using a multi-compound-specific isotope labeling technique ( 200 Hg II , Me 198 Hg, and 202 Hg 0 ). In addition to Hg II methylation and MeHg demethylation, this study revealed that microbially mediated reduction of Hg II , methylation of Hg 0 , and oxidative demethylation-reduction of MeHg occurred under dark conditions; these processes served to transform Hg between different species (Hg 0 , Hg II , and MeHg) in flooded paddy soils. Rapid redox recycling of Hg species contributed to Hg speciation resetting, which promoted the transformation between Hg 0 and MeHg by generating bioavailable Hg II for fuel methylation. Sulfur input also likely affected the microbial community structure and functional profile of Hg II methylators and, therefore, influenced Hg II methylation. The findings of this study contribute to our understanding of Hg transformation processes in paddy soils and provide much-needed knowledge for assessing Hg risks in hydrological fluctuation-regulated ecosystems.

Past and present anthropogenic mercury (Hg) release to ecosystems causes neurotoxicity and cardiovascular disease in humans with an estimated economic cost of $117 billion USD annually. Humans are primarily exposed to Hg via the consumption of contaminated freshwater and marine fish. The UNEP Minamata Convention on Hg aims to curb Hg release to the environment and is accompanied by global Hg monitoring efforts to track its success. The biogeochemical Hg cycle is a complex cascade of release, dispersal, transformation and bio-uptake processes that link Hg sources to Hg exposure. Global change interacts with the Hg cycle by impacting the physical, biogeochemical and ecological factors that control these processes. In this review we examine how global change such as biome shifts, deforestation, permafrost thaw or ocean stratification will alter Hg cycling and exposure. Based on past declines in Hg release and environmental levels, we expect that future policy impacts should be distinguishable from global change effects at the regional and global scales., (© 2023. The Author(s).)

The glymphatic system is the subject of numerous pieces of research in biology. Mathematical modelling plays a considerable role in this field since it can indicate the possible physical effects of this system and validate the biologists' hypotheses. The available mathematical models that describe the system at the scale of the brain (i.e. the macroscopic scale) are often solely based on the diffusion equation and do not consider the fine structures formed by the perivascular spaces. We therefore propose a mathematical model representing the time and space evolution of a mixture flowing through multiple compartments of the brain. We adopt a macroscopic point of view in which the compartments are all present at any point in space. The equations system is composed of two coupled equations for each compartment: One equation for the pressure of a fluid and one for the mass concentration of a solute. The fluid and solute can move from one compartment to another according to certain membrane conditions modelled by transfer functions. We propose to apply this new modelling framework to the clearance of 14C-inulin from the rat brain., Competing Interests: The authors have declared that no competing interests exist., (Copyright: © 2023 Poulain et al. This is an open access article distributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.)

The host spectrum of viruses is quite diverse, as they can sustainedly infect a few species to several phyla. When confronted with a new host, a virus may even infect it and transmit sustainably in this new host, a process called 'viral spillover'. However, the risk of such events is difficult to quantify. As climate change is rapidly transforming environments, it is becoming critical to quantify the potential for spillovers. To address this issue, we resorted to a metagenomics approach and focused on two environments, soil and lake sediments from Lake Hazen, the largest High Arctic freshwater lake in the world. We used DNA and RNA sequencing to reconstruct the lake's virosphere in both its sediments and soils, as well as its range of eukaryotic hosts. We then estimated the spillover risk by measuring the congruence between the viral and the eukaryotic host phylogenetic trees, and show that spillover risk increases with runoff from glacier melt, a proxy for climate change. Should climate change also shift species range of potential viral vectors and reservoirs northwards, the High Arctic could become fertile ground for emerging pandemics.

This study aims to investigate methylmercury (MeHg) demethylation processes in human gut. Here, we determined the compositions and MeHg demethylation rates of gut microbiota in residents from different Hg exposure levels (Wanshan (WS) town and Yangtou (YT) town) and different Hg exposure sources (Zhuchang (ZC) town and YT town) regions. MeHg and inorganic Hg exposure levels in residents of WS town were significantly higher than those of YT and ZC town. Desulfovibrio and Methanogens, which related to Hg methylation/demethylation, showed significantly higher abundance in WS and ZC, comparing with YT. In vitro experiments demonstrated that human intestinal microbiota could degrade MeHg directly. Besides, gut microbiota in WS and ZC exhibited significantly higher demethylation rates than YT, suggesting Desulfovibrio and Methanogens may play important roles in intestinal MeHg demethylation. This study highlights Hg exposure levels and sources may affect demethylation efficiency of gut microbiota, which provides new insights for MeHg demethylation processes in human body., (© 2022. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

The contamination of lakes by industrial emissions is an issue of international concern. Traditional paleolimnology examines sedimentary micro-fossils to infer the biological response to natural and anthropogenic stressors over time. Here, we calculate a theoretical biological effect for historic sediment sections using Probable Effect Concentration Quotient (PEC-Q) and arsenic specific quotient methods and develop novel time-constrained sediment toxicity test methods using a cultured Daphnia sp. combined with a whole cell microbial biosensor to assess the toxicity of past industrial contamination with modern testing methods. These methods were developed using sediments collected from Pocket Lake (Northwest Territories, Canada), a lake known to have exhibited a significant ecological shift following input from nearby gold smelter emissions during the mid 20th century. We then applied these methods to near-, mid-, and far-field sites to assess the response of Daphnia sp. to varying contaminant load. Daphnia sp. mortality exposed to dated sediments indicated a strong concordance with the timing of mining activities, and a strong concordance with PEC-Q and arsenic specific toxicity quotients. In contrast, a decrease in Daphnia mortality was observed during pre-, and post-mining periods when the contaminant burden was lower. Initial assessments of bioavailability using a microbial biosensor indicated that arsenic in porewater is 72-96% bioavailable, and limited evidence that oxidative stress may contribute to the Daphnia sp. toxic response. These results indicate that lake sediment archives can be used to infer missing biomonitoring data in sites of legacy anthropogenic influence, which will be useful for those seeking to conduct cost-effective and efficient preliminary environmental risk assessments., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Microbe-mediated transformations of arsenic (As) often require As to be taken up into cells prior to enzymatic reaction. Despite the importance of these microbial reactions for As speciation and toxicity, understanding of how As bioavailability and uptake are regulated by aspects of extracellular water chemistry, notably dissolved organic matter (DOM), remains limited. Whole-cell biosensors utilizing fluorescent proteins are increasingly used for high-throughput quantification of the bioavailable fraction of As in water. Here, we present a mathematical framework for interpreting the time series of biosensor fluorescence as a measure of As uptake kinetics, which we used to evaluate the effects of different forms of DOM on uptake of trivalent arsenite. We found that thiol-containing organic compounds significantly inhibited uptake of arsenite into cells, possibly through the formation of aqueous complexes between arsenite and thiol ligands. While there was no evidence for competitive interactions between arsenite and low-molecular-weight neutral molecules (urea, glycine, and glyceraldehyde) for uptake through the aquaglyceroporin channel GlpF, which mediates transport of arsenite across cell membranes, there was evidence that labile DOM fractions may inhibit arsenite uptake through a catabolite repression-like mechanism. The observation of significant inhibition of arsenite uptake at DOM/As ratios commonly encountered in wetland pore waters suggests that DOM may be an important control on the microbial uptake of arsenite in the environment, with aspects of DOM quality playing an important role in the extent of inhibition. IMPORTANCE The speciation and toxicity of arsenic in environments like rice paddy soils and groundwater aquifers are controlled by microbe-mediated reactions. These reactions often require As to be taken up into cells prior to enzymatic reaction, but there is limited understanding of how microbial arsenic uptake is affected by variations in water chemistry. In this study, we explored the effect of dissolved organic matter (DOM) quantity and quality on microbial As uptake, with a focus on the role of thiol functional groups that are well known to form aqueous complexes with arsenic. We developed a quantitative framework for interpreting fluorescence time series from whole-cell biosensors and used this technique to evaluate effects of DOM on the rates of microbial arsenic uptake. We show that thiol-containing compounds significantly decrease rates of As uptake into microbial cells at environmentally relevant DOM/As ratios, revealing the importance of DOM quality in regulating arsenic uptake, and subsequent biotransformation, in the environment.

Soil microbial communities are critical for maintaining terrestrial ecosystems and fundamental ecological processes. Mercury (Hg) is a heavy metal that is toxic to microorganisms, but its effects on microbial community assembly and ecosystem multifunctionality in rice paddy ecosystems remain largely unknown. In the current study, we analyzed the microbial community structure and ecosystem multifunctionality of paddy soils across a Hg contamination gradient. The results demonstrated that Hg contamination significantly altered the microbial community structure. The microbial communities were predominantly driven by deterministic selection rather than stochastic processes. The random forest model and variation partition analysis demonstrated that the Hg level was the most important predictor of microbial profiles. Ecosystem multifunctionality decreased across the Hg concentration gradient, and multifunctionality was significantly correlated with soil biodiversity, suggesting that Hg-induced reductions in soil biodiversity led to reduced ecosystem services. A structural equation model showed that Hg contamination directly and indirectly affected ecosystem multifunctionality. The present work broadens our knowledge of the assembly of the microbiome in rice paddies across a Hg contamination gradient and highlights the significance of soil biodiversity in regulating ecosystem functions, especially in Hg-polluted rice paddies., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Methylmercury is a potent neurotoxin that biomagnifies through food webs and which production depends on anaerobic microbial uptake of inorganic mercury (Hg) species. One outstanding knowledge gap in understanding Hg methylation is the nature of bioavailable Hg species. It has become increasingly obvious that Hg bioavailability is spatially diverse and temporally dynamic but current models are mostly built on single thiolated ligand systems, omitting ligand exchanges and interactions, or the inclusion of dissolved gaseous phases. In this study, we used a whole-cell anaerobic biosensor to determine the role of a mixture of thiolated ligands on Hg bioavailability. Serendipitously, we discovered how the diffusion of trace amounts of exogenous biogenic H 2 S, originating from anaerobic microbial ligand degradation, can alter Hg speciation - away from H 2 S production site - to form bioavailable species. Regardless of its origins, H 2 S stands as a mobile mediator of microbial Hg metabolism, connecting spatially separated microbial communities. At a larger scale, global planetary changes are expected to accelerate the production and mobilization of H 2 S and Hg, possibly leading to increased production of the potent neurotoxin; this work provides mechanistic insights into the importance of co-managing biogeochemical cycle disruptions., (© 2022 Society for Applied Microbiology and John Wiley & Sons Ltd.)

Social bee gut microbiotas play key roles in host health and performance. Worryingly, a growing body of literature shows that pesticide exposure can disturb these microbiotas. Most studies examine changes in taxonomic composition in Western honey bee (Apis mellifera) gut microbiotas caused by insecticide exposure. Core bee gut microbiota taxa shift in abundance after exposure but are rarely eliminated, with declines in Bifidobacteriales and Lactobacillus near melliventris abundance being the most common shifts. Pesticide concentration, exposure duration, season and concurrent stressors all influence whether and how bee gut microbiotas are disturbed. Also, the mechanism of disturbance-i.e. whether a pesticide directly affects microbial growth or indirectly affects the microbiota by altering host health-likely affects disturbance consistency. Despite growing interest in this topic, important questions remain unanswered. Specifically, metabolic shifts in bee gut microbiotas remain largely uninvestigated, as do effects of pesticide-disturbed gut microbiotas on bee host performance. Furthermore, few bee species have been studied other than A. mellifera, and few herbicides and fungicides have been examined. We call for these knowledge gaps to be addressed so that we may obtain a comprehensive picture of how pesticides alter bee gut microbiotas, and of the functional consequences of these changes., (© The Author(s) 2022. Published by Oxford University Press on behalf of FEMS.)

Microbial bioreporters provide direct insight into cellular processes by producing a quantifiable signal dictated by reporter gene expression. The core of a bioreporter is a genetic circuit in which a reporter gene (or operon) is fused to promoter and regulatory sequences that govern its expression. In this study, we develop a system for constructing novel Escherichia coli bioreporters based on Golden Gate assembly, a synthetic biology approach for the rapid and seamless fusion of DNA fragments. Gene circuits are generated by fusing promoter and reporter sequences encoding yellow fluorescent protein, mCherry, bacterial luciferase, and an anaerobically active flavin-based fluorescent protein. We address a barrier to the implementation of Golden Gate assembly by designing a series of compatible destination vectors that can accommodate the assemblies. We validate the approach by measuring the activity of constitutive bioreporters and mercury and arsenic biosensors in quantitative exposure assays. We also demonstrate anaerobic quantification of mercury and arsenic in biosensors that produce flavin-based fluorescent protein, highlighting the expanding range of redox conditions that can be examined by microbial bioreporters. IMPORTANCE Microbial bioreporters are versatile genetic tools with wide-ranging applications, particularly in the field of environmental toxicology. For example, biosensors that produce a signal output in the presence of a specific analyte offer less costly alternatives to analytical methods for the detection of environmental toxins such as mercury and arsenic. Biosensors of specific toxins can also be used to test hypotheses regarding mechanisms of uptake, toxicity, and biotransformation. In this study, we develop an assembly platform that uses a synthetic biology technique to streamline construction of novel Escherichia coli bioreporters that produce fluorescent or luminescent signals either constitutively or in response to mercury and arsenic exposure. Beyond the synthesis of novel biosensors, our assembly platform can be adapted for numerous applications, including labeling bacteria for fluorescence microscopy, developing gene expression systems, and modifying bacterial genomes.

Rice consumption is the major pathway for human methylmercury (MeHg) exposure in inland China, especially in mercury (Hg) contaminated regions. MeHg production, a microbially driven process, depends on both the chemical speciation of inorganic divalent mercury, Hg(II), that determines Hg bioavailability for methylation. Studies have shown that Hg(II) speciation in contaminated paddy soils is mostly controlled by natural organic matter and sulfide levels, which are typically thought to limit Hg mobility and bioavailability. Yet, high levels of MeHg are found in rice, calling for reconsideration of the nature of Hg species bioavailable to methylators in paddy soils. Here, we conducted incubation experiments using a multi-isotope tracer technique including 198 Hg(NO 3 ) 2 , natural organic matter bond Hg(II) (NOM- 199 Hg(II)), ferrous sulfide sorbed Hg(II) (≡FeS- 200 Hg(II)), and nanoparticulate mercuric sulfide (nano- 202 HgS), to investigate the relative importance of geochemically diverse yet relevant Hg(II) species on Hg methylation in paddy soils across a Hg concentration gradient. We show that methylation rates for all Hg(II) species tested decreased with increasing Hg concentrations, and that methylation rates using NOM- 199 Hg(II) and nano- 202 HgS as substrates were similar or greater than rates obtained using the labile 198 Hg(NO 3 ) 2 substrate. ≡FeS- 200 Hg(II) yielded the lowest methylation rate in all sites, and thus the formation of FeS is likely a sink for labile 198 Hg(NO 3 ) 2 in sulfide-rich paddy soils. Moreover, the variability in the methylation data for a given site (1 to 5-fold variation depending on the Hg species) was smaller than what was observed across the Hg concentration gradient (10 3 -10 4 fold variation between sites). These findings emphasize that at broad spatial scales, site-specific characteristics, such as microbial community structure, need to be taken into consideration, alongside the nature of the Hg substrate available for methylation, to determine net MeHg production. This study highlights the importance of developing site-specific strategies for remediating Hg pollution., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Mercury (Hg) is a global pollutant and potent neurotoxin that bioaccumulates in food webs as monomethylmercury (MeHg). The production of MeHg is driven by anaerobic and Hg redox cycling pathways, such as Hg reduction, which control the availability of Hg to methylators. Anaerobes play an important role in Hg reduction in methylation hot spots, yet their contributions remain underappreciated due to how challenging these pathways are to study in the absence of dedicated genetic targets and low levels of Hg 0 in anoxic environments. In this study, we used Hg stable isotope fractionation to explore Hg reduction during anoxygenic photosynthesis and fermentation in the model anaerobe Heliobacterium modesticaldum Ice1. We show that cells preferentially reduce lighter Hg isotopes in both metabolisms, leading to mass-dependent fractionation, but mass-independent fractionation commonly induced by UV-visible light is absent. Due to the variability associated with replicate experiments, we could not discern whether dedicated physiological processes drive Hg reduction during photosynthesis and fermentation. However, we demonstrate that fractionation is affected by the interplay between pathways controlling Hg recruitment, accessibility, and availability alongside metabolic redox reactions. The combined contributions of these processes lead to isotopic enrichment during anoxygenic photosynthesis that is in between the values reported for anaerobic respiratory microbial Hg reduction and abiotic photoreduction. Isotope enrichment during fermentation is closer to what has been observed in aerobic bacteria that reduce Hg through dedicated detoxification pathways. Our work suggests that similar controls likely underpin diverse microbe-mediated Hg transformations that affect Hg's fate in oxic and anoxic habitats. IMPORTANCE Anaerobic and photosynthetic bacteria that reduce mercury affect mercury delivery to microbes in methylation sites that drive bioaccumulation in food webs. Anaerobic mercury reduction pathways remain underappreciated in the current view of the global mercury cycle because they are challenging to study, bearing no dedicated genetic targets to establish physiological mechanisms. In this study, we used stable isotopes to characterize the physiological processes that control mercury reduction during photosynthesis and fermentation in the model anaerobe Heliobacterium modesticaldum Ice1. The sensitivity of isotope analyses highlighted the subtle contribution of mercury uptake to the isotope signature associated with anaerobic mercury reduction. When considered alongside the isotope signatures associated with microbial pathways for which genetic determinants have been identified, our findings underscore the narrow range of isotope enrichment that is characteristic of microbial mercury transformations. This suggests that there are common atomic-level controls for biological mercury transformations across a broad range of geochemical conditions.

Motivated by experimental observations in 3D/organoid cultures derived from glioblastoma, we propose a novel mechano-transduction mechanism where the introduction of a chemotherapeutic treatment induces mechanical changes at the cell level. We analyse the influence of these individual mechanical changes on the properties of the aggregates obtained at the population level. We employ a nonlinear volume-filling chemotactic system of partial differential equations, where the elastic properties of the cells are taken into account through the so-called squeezing probability, which depends on the concentration of the treatment in the extracellular microenvironment. We explore two scenarios for the effect of the treatment: first, we suppose that the treatment acts only on the mechanical properties of the cells and, in the second one, we assume it also prevents cell proliferation. We perform a linear stability analysis which enables us to identify the ability of the system to create patterns and fully characterize their size. Moreover, we provide numerical simulations in 1D and 2D that illustrate the shrinking of the aggregates due to the presence of the treatment., (© 2021. The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.)

Smelting activities at Giant Mine (Yellowknife, NWT, Canada) have resulted in high sulfate and arsenic concentrations in nearby lakes. Here we tested whether historic smelting affects current mercury (Hg) cycling in 35 freshwater lakes over a 2800 km 2 area around the former gold mine. We sampled lake water and sediment over three consecutive years (2015-2017) using a factorial sampling design that accounted for different environmental variables known to affect the net methylmercury (MeHg) levels in water. Stable Hg(ii) and MeHg isotope tracers were used to quantify Hg methylation and demethylation rate constants in sediments, and 16S rRNA gene amplicon sequencing was used to characterize microbial community structure. This study reveals that the fraction of methylated total Hg (% MeHg) found in surface water is positively correlated to the sulfate gradient, while the rate at which Hg is methylated (K m ) in sediments is negatively correlated with total arsenic, and positively correlated with dissolved organic carbon, total phosphorous, and % MeHg in the water. Furthermore, 6 of the 28 lakes that had detectable demethylation rate constants (K d ) also had significantly lower DOC concentrations than lakes with non-detectable K d. Our results also show that legacy pollution from smelting activities is affecting the structure of microbial communities in lake sediments. This study reveals the complex dynamics of Hg cycling in this northern environment, highlighting the importance of large-scale studies in which the effect of multiple pollution gradients (e.g. arsenic and sulfate) must be taken into consideration.

Sediment lyophilization is a common process that allows for long-term conservation and sharing of marine sediments for multiple downstream analyses. Although it is often used for geochemical studies, the effects of lyophilization on prokaryotic taxonomic diversity assessment remained to be assessed. Here, we tested the effect of lyophilization on microbial diversity assessment using three sediment layers corresponding to various sediment ages and chemical contamination levels sampled from a marine Mediterranean harbor. Duplicate DNA samples were extracted from wet frozen or lyophilized sediments, and 16S rRNA gene amplicon sequence variants were analyzed. We detected changes in community structure over depth linked to both dominant and less abundant taxa whether sediments were lyophilized or not. Data from both wet frozen and lyophilized sediments led us to conclude that historical chemical contamination of the sediment of Toulon Bay did not appear to be the main environmental variable shaping prokaryotic community structure on the vertical dimension, but that sediment diagenesis was. We conclude that sediment lyophilization is compatible with marine biogeochemical and ecotoxicological studies but that caution should be used when discussing small variations among samples., Competing Interests: Alexandre Poulain is an Academic Editor for PeerJ, (© 2021 Misson et al.)

The Alberta Oil Sands Region in Canada is home to one of the largest oil bitumen deposits in the world. The North American river otter (Lontra canadensis) is a top predator with a small home range and is sensitive to disturbances; it has been designated as a sentinel species for the potential impacts of the natural resource exploitation on freshwater ecosystems in the Alberta Oil Sands Region. With an increasing interest in noninvasive biomarkers, recent studies suggest that gut microbiota can be used as a potential biomarker of early biological effects on aquatic wildlife. The goal of the present study was to determine the river otter gut microbial structure related to environmental variables characterizing mining activities and metal body burden. We obtained 18 trapped animals from and surrounding the surface mineable area of the Alberta Oil Sands Region. The gut microbial community structure was characterized using high-throughput sequencing of 16S rRNA gene amplicon analyses. Trace metal concentrations in the liver were measured by inductively coupled plasma-mass spectrometry. Our study revealed that the gut bacteria of river otters in the Alberta Oil Sands Region clustered in 4 groups dominated by Peptostreptococcaceae, Carnobacteriaceae, Enterobacteriaceae, Clostridiaceae, and Nostocaceae. We show that arsenic, barium, rubidium, liver-body weight ratio, and δ 15 N were associated with each cluster. When comparing affected versus less affected sites, we show that river otter gut bacterial community and structure are significantly related to trophic level of the river otter but not to Alberta Oil Sands Region mining activities. Our study reveals that the gut bacterial dynamics can provide insights into the diet and habitat use of river otters but that more work is needed to use it as a pollution biomarker. Environ Toxicol Chem 2020;39:2516-2526. © 2020 SETAC., (© 2020 SETAC.)

The widely accepted conceptual model of mercury (Hg) cycling in freshwater lakes (atmospheric deposition and runoff of inorganic Hg, methylation in bottom sediments and subsequent bioaccumulation and biomagnification in biota) is practically accepted as common knowledge. There is mounting evidence that the dominant processes that regulate inputs, transformations, and bioavailability of Hg in many lakes may be missing from this picture, and the fixation on the temperate stratified lake archetype is impeding our exploration of understudied, but potentially important sources of methylmercury to freshwater lakes. In this review, the importance of understudied biogeochemical processes and sites of methylmercury production are highlighted, including the complexity of redox transformations of Hg within the lake system itself, the complex assemblage of microbes found in biofilms and periphyton (two vastly understudied important sources of methylmercury in many freshwater ecosystems), and the critical role of autochthonous and allochthonous dissolved organic matter which mediates the net supply of methylmercury from the cellular to catchment scale. A conceptual model of lake Hg in contrasting lakes and catchments is presented, highlighting the importance of the autochthonous and allochthonous supply of dissolved organic matter, bioavailable inorganic mercury and methylmercury and providing a framework for future convergent research at the lab and field scales to establish more mechanistic process-based relationships within and among critical compartments that regulate methylmercury concentrations in freshwater ecosystems., Competing Interests: Declaration of competing interest The authors declare no conflict of interest., (Copyright © 2020 Elsevier B.V. All rights reserved.)

Rice paddies are agricultural sites of special concern because the potent toxin methylmercury (MeHg), produced in rice paddy soils, accumulates in rice grains. MeHg cycling is mostly controlled by microbes but their importance in MeHg production and degradation in paddy soils and across a Hg concentration gradient remains unclear. Here we used surface and rhizosphere soil samples in a series of incubation experiments in combination with stable isotope tracers to investigate the relative importance of different microbial groups on MeHg production and degradation across a Hg contamination gradient. We showed that sulfate reduction was the main driver of MeHg formation and concentration at control sites, and that methanogenesis had an important and complex role in MeHg cycling as Hg concentrations increased. The inhibition of methanogenesis at the mining sites led to an increase in MeHg production up to 16.6-fold and a decrease in MeHg degradation by up to 77%, suggesting that methanogenesis is associated with MeHg degradation as Hg concentrations increased. This study broadens our understanding of the roles of microbes in MeHg cycling and highlights methanogenesis as a key control of MeHg concentrations in rice paddies, offering the potential for mitigation of Hg contamination and for the safe production of rice in Hg-contaminated areas.

Temperatures in the Arctic are expected to increase dramatically over the next century, and transform high latitude watersheds. However, little is known about how microbial communities and their underlying metabolic processes will be affected by these environmental changes in freshwater sedimentary systems. To address this knowledge gap, we analyzed sediments from Lake Hazen, NU Canada. Here, we exploit the spatial heterogeneity created by varying runoff regimes across the watershed of this uniquely large high-latitude lake to test how a transition from low to high runoff, used as one proxy for climate change, affects the community structure and functional potential of dominant microbes. Based on metagenomic analyses of lake sediments along these spatial gradients, we show that increasing runoff leads to a decrease in taxonomic and functional diversity of sediment microbes. Our findings are likely to apply to other, smaller, glacierized watersheds typical of polar or high latitude ecosystems; we can predict that such changes will have far reaching consequences on these ecosystems by affecting nutrient biogeochemical cycling, the direction and magnitude of which are yet to be determined., (Copyright © 2020 Colby, Ruuskanen, St.Pierre, St.Louis, Poulain and Aris-Brosou.)

Mine tailings are found worldwide and can have significant impacts on ecosystem and human health. In this study, natural vegetation patterns on arsenical (As) gold (Au) mine tailings located in Sudbury, Ontario were assessed using transects located at the edge of the tailings and on the tailings. Vegetation communities were significantly different between the edge and open tailings areas of the site. Arsenic concentrations in both areas were extremely variable (from 285-17,567 mg/kg) but were not significantly correlated with vegetation diversity at the site. Nutrients (carbon (C), phosphorus (P)) and organic matter concentrations were associated with higher diversity and with the presence of climax vegetation on the tailings, but there were no significant relationships between tailings chemistry and vegetation indices on the edge. Encroachment onto the tailings from the edge occurred in conventional succession patterns, with a clear gradient from grasses (Agrostis gigantea) to trees such as Picea glauca. On the tailings, a nucleation pattern was visible, distinct from conventional succession. Trees and shrubs such as Betula papyrifera and Diervilla lonicera were associated with higher diversity and higher nutrient concentrations in the underlying tailings, whereas grasses such as A. gigantea were not. We concluded that at all areas of the site, vegetation - particularly trees - was facilitating amelioration of the underlying tailings. Despite high concentrations of As, nutrients appeared to have a greater influence than metals on vegetation diversity., Competing Interests: Declaration of interests The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

The presence of arsenic in irrigation and drinking waters is a threat to worldwide human health. Dissolved organic matter (DOM) is a ubiquitous and photoreactive sorbent of arsenic, capable of both suppressing and enhancing its mobility. Microbes can control the mobilization of mineral-bound arsenic, through redox processes thought to occur intracellularly. The role that DOM plays on the bioavailability of arsenic to microbes is often invoked but remains untested experimentally. Here, using a whole-cell biosensor, we tested the role of DOM on As(III) and As(V) bioavailability. Using cation amendments, we explored the nature of As-DOM interactions. We found As bioavailability to be dependent on [As]/[DOM] ratio and on the strength of As binding to DOM which varied as a function of time. We further tested the role of DOM on As(III) photooxidation and showed that As(III) photooxidation rate is limited by the strength of its interactions with DOM and sensitive to ionic competitive desorption. Our study demonstrates the dynamic control that photoreactive DOM poses on the bioavailability and reactivity of As in the environment and highlights the kinetic controls that DOM can possibly exert on As toxicity at various levels in foodwebs., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier B.V. All rights reserved.)

Anthropogenic mercury remobilization has considerably increased since the Industrial Revolution in the late 1700s. The Minamata Convention on Mercury is a United Nations treaty (2017) aiming at curbing mercury emissions. Unfortunately, evaluating the effectiveness of such a global treaty is hampered by our inability to determine the lag in aquatic ecosystem responses to a change in atmospheric mercury deposition. Whereas past metal concentrations are obtained from core samples, there are currently no means of tracking historical metal bioavailability or toxicity. Here, we recovered DNA from nine dated sediment cores collected in Canada and Finland, and reconstructed the past demographics of microbes carrying genes coding for the mercuric reductase (MerA)-an enzyme involved in Hg detoxification-using Bayesian relaxed molecular clocks. We found that the evolutionary dynamics of merA exhibited a dramatic increase in effective population size starting from 1783.8 ± 3.9 CE, which coincides with both the Industrial Revolution, and with independent measurements of atmospheric Hg concentrations. We show that even low levels of anthropogenic mercury affected the evolutionary trajectory of microbes in the Northern Hemisphere, and that microbial DNA encoding for detoxification determinants stored in environmental archives can be used to track historical pollutant toxicity.

In the latter half of the 1950s, a large amount of methylmercury (MeHg) was discharged directly into Minamata Bay, Japan by a chemical factory, resulting in the contamination of the fish and shellfish. Ultimately, an outbreak of MeHg intoxication, called Minamata disease, occurred. From 1977 to 1988, the Kumamoto Prefectural Government dredged and transferred sediments exceeding 25 μg/g of total mercury (THg, dry basis) into a strictly segregated area of the bay near the wastewater outlet, then this area was landfilled. We conducted analyses of the mercury speciation in preserved Minamata Bay sludge samples (collected from inside of the bay prior to the termination of the remediation project; n=4) and recent Minamata Bay sediments (collected outside the dredging area of the bay; n=5) to evaluate the potential risk of the sludge/sediment leakage from the reclaimed land to the Minamata Bay. Median THg (dry basis) concentrations were 241 μg/g for the preserved sludge, 6.1 μg/g for the recent Minamata Bay sediments, and 0.18 μg/g for a single control sample; median MeHg concentrations (percentage of MeHg in THg) were 108 ng/g (0.031%), 3.7 ng/g (0.12%), and 0.71 ng/g (0.41%), respectively. In all the samples, the MeHg% decreased exponentially with increasing THg concentration. The extractability of THg from each sample into seawater was shown to be much lower than that of MeHg. The extracted MeHg was 0.86% for the preserved sludge, 4.57% for the recent Minamata Bay sediments, and 7.89% for the control. The predominant chemical form of mercury in the preserved sludge containing the highest THg concentration was found to be stable β-mercury sulfide (HgS) based on transmission electron microscopy linked with energy-dispersive X-ray spectroscopy (TEM-EDX) and X-ray absorption fine structure (XAFS) analyses., (Copyright © 2019 Elsevier Inc. All rights reserved.)

The consumption of rice has become a global food safety issue because rice paddies support the production of high levels of the potent neurotoxin, methylmercury. The production of methylmercury is carried out by chemotrophic anaerobes that rely on a diversity of terminal electron acceptors, namely sulphate. Sulphur can be a limiting nutrient in rice paddies, and sulphate amendments are often used to stimulate crop production, which can increase methylmercury production. Mercury (Hg) redox cycling can affect Hg methylation by controlling the delivery of inorganic Hg substrates to methylators in anoxic habitats. Whereas sulphur is recognized as a key substrate controlling methylmercury production, the controls sulphur exerts on other microbe-mediated Hg transformations remain poorly understood. To explore the potential coupling between sulphur assimilation and anaerobic Hg II reduction to Hg 0 , we studied Heliobacillus mobilis, a mesophilic anoxygenic phototroph representative from the Heliobacteriacea family originally isolated from a rice paddy. Here, we tested whether the redox state of the sulphur sources available to H. mobilis would affect its ability to reduce Hg II . By comparing Hg 0 production over a redox gradient of sulphur sources, we demonstrate that phototrophic Hg II reduction is favoured in the presence of reduced sulphur sources such as thiosulphate and cysteine. We also show that cysteine exerts dynamic control on Hg cycling by affecting not only Hg's bioavailability but also its abiotic photoreduction under low light conditions. Specifically, in the absence of cells we show that organic matter (as yeast extract) and cysteine are both required for photoreduction to occur. This study offers insights into how one of the most primitive forms of photosynthesis affects Hg redox transformations and frames Heliobacteria as key players in Hg cycling within paddy soils, forming a basis for management strategies to mitigate Hg accumulation in rice., (© 2019 John Wiley & Sons Ltd.)

Improper design and maintenance of stormwater ponds (SWPs) may lead to hypoxic conditions, poor water quality and the production of hydrogen sulfide (H 2 S). The objective of this study is to develop a comprehensive understanding of hypoxic conditions of SWPs, with a focus on the potential for H 2 S production and emission. This study was conducted at two retention SWPs in Ottawa, Canada; a problematic pond with the propensity for H 2 S emission and a reference pond that did not demonstrate H 2 S emission. The investigation illustrated a significant impact of low dissolved oxygen (DO) concentrations, hypoxic conditions, on the concentration of total sulfides in the water column. Both ponds were shown to periodically experience hypoxic conditions at depth, especially during summer periods with less precipitation and across longer periods of winter, ice-covered conditions. The problem pond, however, was shown to experience lower DO and longer hypoxic conditions than the reference pond in both non-ice-covered and ice-covered conditions due to greater depth and a longer hydraulic retention time. Hypoxic conditions were initiated at the deepest locations in the problem pond and subsequently were spread across the entirety of the pond under winter, ice-covered conditions. Algal biomass (Chlorophyll-a) and soluble biochemical oxygen demand concentrations were shown to not likely be significant factors in the development of hypoxia in the H 2 S-generating pond. Algal blooms of colonial Chrysophyceae, Synura, a known mixotroph, were observed during ice-covered conditions in the problem pond possibly due to stress-coping mechanisms of algae.

The biological mobilization of mercury (Hg) into microbes capable of Hg methylation is one of the limiting steps in the formation of the neurotoxin methylmercury (MeHg). Although algal dissolved organic matter (DOM) has been associated with increased MeHg production, the relationship between bacterial Hg uptake and algal DOM remains unexplored. In this study, we aimed to address how the quantity and quality of DOM, freshly harvested from several algae, affected the bacterial uptake of Hg with the use of a biosensor capable of functioning both aerobically and anaerobically. We combined biosensor measurements with high-resolution mass spectrometry and field-flow fractionation to elucidate how DOM composition and molecular weight influenced microbial Hg uptake. We showed that freshly harvested DOM from Chlorophyte and Euglena mutabilis strongly inhibited aerobic and anaerobic Hg uptake, whereas DOM harvested from Euglena gracilis did not exhibit this same pronounced effect. Once fractionated, we found that amino acids and polyamines, most abundant in Euglena gracilis DOM, were positively correlated to increase Hg uptake, suggesting that these molecules are potentially underappreciated ligands affecting Hg bioavailability. As water quality is affected by eutrophication, algal community assemblages will change, leading to variations in the nature of autochthonous DOM released in aquatic systems. Our results highlight that variations in the emergent properties of DOM originating from varying algal species can have a profound effect on bacterial Hg uptake and thus methylation.

Mercury (Hg) bioavailability to microbes is a key step to toxic Hg biomagnification in food webs. Cadmium (Cd) transformations and bioavailability to bacteria control the amount that will accumulate in staple food crops. The bioavailability of these metals is dependent on their speciation in solution, but more particularly under anoxic conditions where Hg is methylated to toxic monomethylmercury (MeHg) and Cd persists in the rhizosphere. Whole-cell microbial biosensors give a quantifiable signal when a metal enters the cytosol and therefore are useful tools to assess metal bioavailability. Unfortunately, most biosensing efforts have so far been constrained to oxic environments due to the limited ability of existing reporter proteins to function in the absence of oxygen. In this study, we present our effort to develop and optimize a whole-cell biosensor assay capable of functioning anaerobically that can detect metals under anoxic condition in quasi-real time and within hours. We describe how the biosensor can help assess how chemical variables relevant to the environmental cycling of metals affect their bioavailability. The following protocol includes methods to (1) prepare Hg and Cd standards under anoxic conditions, (2) prepare the biosensor in the absence of oxygen, (3) design and execute an experiment to determine how a series of variable affects Hg or Cd bioavailability, and (4) to quantify and interpret biosensor data. We show the linear ranges of the biosensors and provide examples showing the method's ability to distinguish between metal bioavailability and toxicity by utilizing both metal-inducible and constitutive strains.

Despite its high toxicity and widespread occurrence in many parts of the world, arsenic (As) concentrations in decentralized water supplies such as domestic wells remain often unquantified. One limitation to effective monitoring is the high cost and lack of portability of current arsenic speciation techniques. Here, we present an arsenic biosensor assay capable of quantifying and determining the bioavailable fraction of arsenic species at environmentally relevant concentrations. First, we found that inorganic phosphate, a buffering agent and nutrient commonly found in most bioassay exposure media, was in fact limiting As(V) uptake, possibly explaining the variability in As(V) detection reported so far. Second, we show that the nature of the carbon source used in the bioassay differentially affects the response of the biosensor to As(III). Finally, our data support the existence of non-specific reduction pathways (non- ars encoded) that are responsible for the reduction of As(V) to As(III), allowing its detection by the biosensor. To validate our laboratory approach using field samples, we performed As(III) and As(V) standard additions on natural water samples collected from 17 lakes surrounding Giant Mine in Yellowknife (NWT), Canada. We found that legacy arsenic contamination in these lake water samples was accurately quantified by the biosensor. Interestingly, bioavailability of freshly added standards showed signs of matrix interference, indicative of dynamic interactions between As(III), As(V) and environmental constituents that have yet to be identified. Our results point toward dissolved organic carbon as possibly controlling these interactions, thus altering As bioavailability.

The Arctic is undergoing rapid environmental change, potentially affecting the physicochemical constraints of microbial communities that play a large role in both carbon and nutrient cycling in lacustrine environments. However, the microbial communities in such Arctic environments have seldom been studied, and the drivers of their composition are poorly characterized. To address these gaps, we surveyed the biologically active surface sediments in Lake Hazen, the largest lake by volume north of the Arctic Circle, and a small lake and shoreline pond in its watershed. High-throughput amplicon sequencing of the 16S rRNA gene uncovered a community dominated by Proteobacteria, Bacteroidetes, and Chloroflexi, similar to those found in other cold and oligotrophic lake sediments. We also show that the microbial community structure in this Arctic polar desert is shaped by pH and redox gradients. This study lays the groundwork for predicting how sediment microbial communities in the Arctic could respond as climate change proceeds to alter their physicochemical constraints.

Wildlife are exposed to neurotoxic mercury at locations distant from anthropogenic emission sources because of long-range atmospheric transport of this metal. In this study, mercury bioaccumulation in insectivorous bat species (Mammalia: Chiroptera) was investigated on a broad geographic scale in Canada. Fur was analyzed (n=1178) for total mercury from 43 locations spanning 20° latitude and 77° longitude. Total mercury and methylmercury concentrations in fur were positively correlated with concentrations in internal tissues (brain, liver, kidney) for a small subset (n=21) of little brown bats (Myotis lucifugus) and big brown bats (Eptesicus fuscus), validating the use of fur to indicate internal mercury exposure. Brain methylmercury concentrations were approximately 10% of total mercury concentrations in fur. Three bat species were mainly collected (little brown bats, big brown bats, and northern long-eared bats [M. septentrionalis]), with little brown bats having lower total mercury concentrations in their fur than the other two species at sites where both species were sampled. On average, juvenile bats had lower total mercury concentrations than adults but no differences were found between males and females of a species. Combining our dataset with previously published data for eastern Canada, median total mercury concentrations in fur of little brown bats ranged from 0.88-12.78μg/g among 11 provinces and territories. Highest concentrations were found in eastern Canada where bats are most endangered from introduced disease. Model estimates of atmospheric mercury deposition indicated that eastern Canada was exposed to greater mercury deposition than central and western sites. Further, mean total mercury concentrations in fur of adult little brown bats were positively correlated with site-specific estimates of atmospheric mercury deposition. This study provides the largest geographic coverage of mercury measurements in bats to date and indicates that atmospheric mercury deposition is important in determining spatial patterns of mercury accumulation in a mammalian species., (Crown Copyright © 2018. Published by Elsevier B.V. All rights reserved.)

We investigated monomethylmercury (MMHg) bioaccumulation in lakes across a 30° latitudinal gradient in eastern Canada to test the hypothesis that climate-related environmental conditions affect the sensitivity of Arctic lakes to atmospheric mercury contamination. Aquatic invertebrates (chironomid larvae, zooplankton) provided indicators of MMHg bioaccumulation near the base of benthic and planktonic food chains. In step with published data showing latitudinal declines in atmospheric mercury deposition in Canada, we observed lower total mercury concentrations in water and sediment of higher latitude lakes. Despite latitudinal declines of inorganic mercury exposure, MMHg bioaccumulation in aquatic invertebrates did not concomitantly decline. Arctic lakes with greater MMHg in aquatic invertebrates either had (1) higher water MMHg concentrations (reflecting ecosystem MMHg production) or (2) low water concentrations of MMHg, dissolved organic carbon (DOC), chlorophyll, and total nitrogen (reflecting lake sensitivity). The MMHg:DOC ratio of surface water was a strong predictor of lake sensitivity to mercury contamination. Bioaccumulation factors for biofilms and seston in Arctic lakes showed more efficient uptake of MMHg in low DOC systems. Environmental conditions associated with low biological production in Arctic lakes and their watersheds increased the sensitivity of lakes to MMHg.

Monomethylmercury (MMHg) is a potent neurotoxicant that can be bioaccumulated and biomagnified through trophic levels. Human populations whose diets contain MMHg are at risk of MMHg toxicity. The gut microbiota was identified as a potential factor causing variation in MMHg absorption and body burden. However, little is known about the role of gut microbiota on Hg transformations. We conducted a series of in vitro experiments to study the effects of dietary nutrient change on Hg metabolism and the human gut microbiota using anoxic fecal slurry incubations. We used stable Hg isotope tracers to track MMHg production and degradation and characterized the microbiota using high throughput sequencing of the 16S rRNA gene. We show that the magnitude of MMHg degradation is individual dependent and rapidly responds to changes in nutrient amendments, leading to complete degradation of the MMHg present. Although the mechanism involved remains unknown, it does not appear to involve the well-known mer operon. Our data are the first to show a nutrient dependency on the ability of the simulated human gut microbiota to demethylate MMHg. This work provides much-needed insights into individual variations in Hg absorption and potential toxicity.

Uranium contamination is a worldwide problem that grows proportionally to human demands for energy and armory. Understanding U cycling in the environment is of eminent interest, mostly concerning ecosystems directly impacted by point sources. In Bow Lake (Ontario, Canada), which is located adjacent to a former U mine, exceptionally high concentrations of U are related to U dispersion from tailings and biogeochemical processes such as biotic reduction and adsorption. This has been shown by a U-Pb isotope composition model. In this study, we use U isotope fractionation (δ 238 U) to highlight U cycling and the role of bacteria (Geobacteraceae and sulfate-reducing bacteria) in affecting U cycling. Bacteria affected U cycling directly via biotic U reduction and indirectly via reductive dissolution of carrier phases. All the processes are interconnected through diagenetic reactions with the supply of bioavailable organic matter being the primary driving force of the diagenesis. This study is the first to use multiple biogeochemical and isotopic approaches to track U cycling from a contamination point source to U storage in lake sediments., (Copyright © 2017 Elsevier B.V. All rights reserved.)

Mercury (Hg) bioavailability to bacteria in marine systems is the first step toward its bioamplification in food webs. These systems exhibit high salinity and ionic strength that will both alter Hg speciation and properties of the bacteria cell walls. The role of Hg speciation on Hg bioavailability in marine systems has not been teased apart from that of ionic strength on cell wall properties, however. We developed and optimized a whole-cell Hg bioreporter capable of functioning under aerobic and anaerobic conditions and exhibiting no physiological limitations of signal production to changes in ionic strength. We show that ionic strength controls the bioavailability of Hg species, regardless of their charge, possibly by altering properties of the bacterial cell wall. The unexpected anaerobic bioavailability of negatively charged halocomplexes may help explain Hg methylation in marine systems such as the oxygen-deficient zone in the oceanic water column, sea ice or polar snow.

Mercury (Hg) is an anthropogenic pollutant that is toxic to wildlife and humans, but the response of remote ecosystems to globally distributed Hg is elusive. Here, we use DNA extracted from a dated sediment core to infer the response of microbes to historical Hg delivery. We observe a significant association between the mercuric reductase gene (merA) phylogeny and the timing of Hg deposition. Using relaxed molecular clock models, we show a significant increase in the scaled effective population size of the merA gene beginning ~200 years ago, coinciding with the Industrial Revolution and a coincident strong signal for positive selection acting on residues in the terminal region of the mercuric reductase. This rapid evolutionary response of microbes to changes in the delivery of anthropogenic Hg indicates that microbial genomes record ecosystem response to pollutant deposition in remote regions.

Contaminants in the Canadian Arctic have been studied over the last twenty years under the guidance of the Northern Contaminants Program. This paper provides the current state of knowledge on mercury (Hg) in the Canadian Arctic terrestrial environment. Snow, ice, and soils on land are key reservoirs for atmospheric deposition and can become sources of Hg through the melting of terrestrial ice and snow and via soil erosion. In the Canadian Arctic, new data have been collected for snow and ice that provide more information on the net accumulation and storage of Hg in the cryosphere. Concentrations of total Hg (THg) in terrestrial snow are highly variable but on average, relatively low (<5 ng L(-1)), and methylmercury (MeHg) levels in terrestrial snow are also generally low (<0.1 ng L(-1)). On average, THg concentrations in snow on Canadian Arctic glaciers are much lower than those reported on terrestrial lowlands or sea ice. Hg in snow may be affected by photochemical exchanges with the atmosphere mediated by marine aerosols and halogens, and by post-depositional redistribution within the snow pack. Regional accumulation rates of THg in Canadian Arctic glaciers varied little during the past century but show evidence of an increasing north-to-south gradient. Temporal trends of THg in glacier cores indicate an abrupt increase in the early 1990 s, possibly due to volcanic emissions, followed by more stable, but relatively elevated levels. Little information is available on Hg concentrations and processes in Arctic soils. Terrestrial Arctic wildlife typically have low levels of THg (<5 μg g(-1) dry weight) in their tissues, although caribou (Rangifer tarandus) can have higher Hg because they consume large amounts of lichen. THg concentrations in the Yukon's Porcupine caribou herd vary among years but there has been no significant increase or decrease over the last two decades., (Copyright © 2014 Elsevier B.V. All rights reserved.)

Sulfate (SO4(2-)) and mercury (Hg) are airborne pollutants transported to the Arctic where they can affect properties of the atmosphere and the health of marine or terrestrial ecosystems. Detecting trends in Arctic Hg pollution is challenging because of the short period of direct observations, particularly of actual deposition. Here, we present an updated proxy record of atmospheric SO4(2-) and a new 40-year record of total Hg (THg) and monomethyl Hg (MeHg) deposition developed from a firn core (P2010) drilled from Penny Ice Cap, Baffin Island, Canada. The updated P2010 record shows stable mean SO4(2-) levels over the past 40 years, which is inconsistent with observations of declining atmospheric SO4(2-) or snow acidity in the Arctic during the same period. A sharp THg enhancement in the P2010 core ca 1991 is tentatively attributed to the fallout from the eruption of the Icelandic volcano Hekla. Although MeHg accumulation on Penny Ice Cap had remained constant since 1970, THg accumulation increased after the 1980s. This increase is not easily explained by changes in snow accumulation, marine aerosol inputs or air mass trajectories; however, a causal link may exist with the declining sea-ice cover conditions in the Baffin Bay sector. The ratio of THg accumulation between pre-industrial times (reconstructed from archived ice cores) and the modern industrial era is estimated at between 4- and 16-fold, which is consistent with estimates from Arctic lake sediment cores. The new P2010 THg record is the first of its kind developed from the Baffin Island region of the eastern Canadian Arctic and one of very few such records presently available in the Arctic. As such, it may help to bridge the knowledge gap linking direct observation of gaseous Hg in the Arctic atmosphere and actual net deposition and accumulation in various terrestrial media., (Copyright © 2014 Elsevier B.V. All rights reserved.)

The Canadian Arctic has vast freshwater resources, and fish are important in the diet of many Northerners. Mercury is a contaminant of concern because of its potential toxicity and elevated bioaccumulation in some fish populations. Over the last decade, significant advances have been made in characterizing the cycling and fate of mercury in these freshwater environments. Large amounts of new data on concentrations, speciation and fluxes of Hg are provided and summarized for water and sediment, which were virtually absent for the Canadian Arctic a decade ago. The biogeochemical processes that control the speciation of mercury remain poorly resolved, including the sites and controls of methylmercury production. Food web studies have examined the roles of Hg uptake, trophic transfer, and diet for Hg bioaccumulation in fish, and, in particular, advances have been made in identifying determinants of mercury levels in lake-dwelling and sea-run forms of Arctic char. In a comparison of common freshwater fish species that were sampled across the Canadian Arctic between 2002 and 2009, no geographic patterns or regional hotspots were evident. Over the last two to four decades, Hg concentrations have increased in some monitored populations of fish in the Mackenzie River Basin while other populations from the Yukon and Nunavut showed no change or a slight decline. The different Hg trends indicate that the drivers of temporal change may be regional or habitat-specific. The Canadian Arctic is undergoing profound environmental change, and preliminary evidence suggests that it may be impacting the cycling and bioaccumulation of mercury. Further research is needed to investigate climate change impacts on the Hg cycle as well as biogeochemical controls of methylmercury production and the processes leading to increasing Hg levels in some fish populations in the Canadian Arctic., (Crown Copyright © 2014. Published by Elsevier B.V. All rights reserved.)

This review summarizes data and information which have been generated on mercury (Hg) in the marine environment of the Canadian Arctic since the previous Canadian Arctic Contaminants Assessment Report (CACAR) was released in 2003. Much new information has been collected on Hg concentrations in marine water, snow and ice in the Canadian Arctic. The first measurements of methylation rates in Arctic seawater indicate that the water column is an important site for Hg methylation. Arctic marine waters were also found to be a substantial source of gaseous Hg to the atmosphere during the ice-free season. High Hg concentrations have been found in marine snow as a result of deposition following atmospheric mercury depletion events, although much of this Hg is photoreduced and re-emitted back to the atmosphere. The most extensive sampling of marine sediments in the Canadian Arctic was carried out in Hudson Bay where sediment total Hg (THg) concentrations were low compared with other marine regions in the circumpolar Arctic. Mass balance models have been developed to provide quantitative estimates of THg fluxes into and out of the Arctic Ocean and Hudson Bay. Several recent studies on Hg biomagnification have improved our understanding of trophic transfer of Hg through marine food webs. Over the past several decades, Hg concentrations have increased in some marine biota, while other populations showed no temporal change. Marine biota also exhibited considerable geographic variation in Hg concentrations with ringed seals, beluga and polar bears from the Beaufort Sea region having higher Hg concentrations compared with other parts of the Canadian Arctic. The drivers of these variable patterns of Hg bioaccumulation, both regionally and temporally, within the Canadian Arctic remain unclear. Further research is needed to identify the underlying processes including the interplay between biogeochemical and food web processes and climate change., (Crown Copyright © 2014. Published by Elsevier B.V. All rights reserved.)

A dynamic mass balance model was developed for the St. Lawrence River near Cornwall, Ontario that predicts and hindcasts mercury concentrations and fluxes in three forms, elemental Hg (Hg(0)), divalent mercury (Hg(2+)), and methyl mercury (MeHg), in a six compartment environment (air, water, porewater, sediment, periphyton, and benthic invertebrates). Our objective was to construct a dynamic mass balance model for mercury in the St. Lawrence River near Cornwall, Ontario based on the framework and results of a steady-state mass balance model developed previously for this site. The second objective was to estimate industrial mercury emissions based on mercury residues deposited in sediments prior to 1970, the year when regulations were implemented to reduce mercury pollution in the environment. We compiled mercury concentrations, fluxes, and transformation rates from previous studies completed in this section of the river (area of approximately 100km(2)) to develop the model. Estimated mercury concentrations in all media were similar to measured data (R(2)=0.99), with only minor exceptions, providing a satisfactory overall description of the mercury loadings and transformation rates of the different mercury species. The estimated historical emissions prior to 1970 from local industries along the Cornwall waterfront were approximately 400kgyear(-1). A storm sewer discharge of 5000m(3)/day resulted in a significant increase in mercury concentrations, particularly in sediment (617ngg(-1) to 624ngg(-1); p=0.004). Model results suggest that discharges of mercury from sources such as local industries and storm sewers have an impact on mercury in media such as sediment and water. This model should provide a basis for predicting and hindcasting mercury concentrations in other river environments as well, because it considers three distinct forms of mercury, and contains environmental media common to all rivers, including some (e.g. periphyton) not typically included in previous mercury models., (Copyright © 2014 Elsevier B.V. All rights reserved.)

Predicting the bioavailability of inorganic mercury (Hg) to bacteria that produce the potent bioaccumulative neurotoxin monomethylmercury remains one of the greatest challenges in predicting the environmental fate and transport of Hg. Dissolved organic matter (DOM) affects mercury methylation due to its influence on cell physiology (as a potential nutrient) and its influence on Hg(II) speciation in solution (as a complexing agent), therefore controlling Hg bioavailability. We assessed the role of DOM on Hg(II) bioavailability to a gram-negative bacterium bioreporter under oxic pseudo- and nonequilibrium conditions, using defined media and field samples spanning a wide range of DOM levels. Our results showed that Hg(II) was considerably more bioavailable under nonequilibrium conditions than when DOM was absent or when Hg(II) and DOM had reached pseudoequilibrium (24 h) prior to cell exposure. Under these enhanced uptake conditions, Hg(II) bioavailability followed a bell shaped curve as DOM concentrations increased, both for defined media and natural water samples, consistent with bioaccumulation results in a companion paper (this issue) observed for amphipods. Experiments also suggest that DOM may not only provide shuttle molecules facilitating Hg uptake, but also alter cell wall properties to facilitate the first steps toward Hg(II) internalization. We propose the existence of a short-lived yet critical time window (<24 h) during which DOM facilitates the entry of newly deposited Hg(II) into aquatic food webs, suggesting that the bulk of mercury incorporation in aquatic food webs would occur within hours following its deposition from the atmosphere.

Dissolved organic carbon (DOC) is known to affect the Hg cycle in aquatic environments due to its overriding influence on complexation, photochemical, and microbial processes, but its role as a mediating factor in the bioaccumulation of Hg in aquatic biota has remained enigmatic. Here, we examined 26 tundra lakes in Canada's western Arctic that span a large gradient of DOC concentrations to show that total Hg (HgT) and methyl mercury (MeHg) accumulation by aquatic invertebrates is defined by a threshold response to Hg-DOC binding. Our results showed that DOC promotes HgT and MeHg bioaccumulation in tundra lakes having low DOC (<8.6 - 8.8 mg C L(-1); DOC threshold concentration, TC) whereas DOC inhibits HgT and MeHg bioaccumulation in lakes having high DOC (>DOC TC), consistent with bioaccumulation results in a companion paper (this issue) using a microbial bioreporter. Chemical equilibrium modeling showed that Hg bioaccumulation factors were elevated when Hg was associated mainly to fulvic acids, but became dramatically reduced when DOC was >8.5 mg C L(-1), at which point Hg was associated primarily with strong binding sites on larger, less bioaccessible humic acids. This study demonstrates that the biological uptake of Hg in lakes is determined by binding thresholds on DOC, a water quality variable predicted to change markedly with future environmental change.

While microbial communities play a key role in the geochemical cycling of nutrients and contaminants in anaerobic freshwater sediments, their structure and activity in polar desert ecosystems are still poorly understood, both across heterogeneous freshwater environments such as lakes and wetlands, and across sediment depths. To address this question, we performed targeted environmental transcriptomics analyses and characterized microbial diversity across three depths from sediment cores collected in a lake and a wetland, located on Cornwallis Island, NU, Canada. Microbial communities were characterized based on 16S rRNA and two functional gene transcripts: mcrA, involved in archaeal methane cycling and glnA, a bacterial housekeeping gene implicated in nitrogen metabolism. We show that methane cycling and overall bacterial metabolic activity are the highest at the surface of lake sediments but deeper within wetland sediments. Bacterial communities are highly diverse and structured as a function of both environment and depth, being more diverse in the wetland and near the surface. Archaea are mostly methanogens, structured by environment and more diverse in the wetland. McrA transcript analyses show that active methane cycling in the lake and wetland corresponds to distinct communities with a higher potential for methane cycling in the wetland. Methanosarcina spp., Methanosaeta spp. and a group of uncultured Archaea are the dominant methanogens in the wetland while Methanoregula spp. predominate in the lake.