An increase in the occurrence of large, high severity wildfires in the western Pacific Northwest (PNW), USA, has created an urgent need for science to better inform forest management and policy decisions to maintain source water quality in the region. The western PNW faces similar challenges to other regions with shifting wildfire regimes and large population centers reliant on surface water from forested catchments. However, the uniquely wet and highly seasonal climate of the western PNW suggests that findings from other, more frequently burned regions may not be directly applicable. To identify science, monitoring, and management gaps and opportunities in the western PNW, this review was collaboratively undertaken by academics, non-government and industry representatives, and local, state, and federal government entities who have been working together since the 2020 Labor Day fires in Oregon. Focusing on Oregon and Washington, we found that monitoring networks for continuous water quantity and quality cover much of the state with greater representation in western U.S. ecoregions, but few studies have analyzed and published these data to capture and communicate the post-wildfire response. Approximately half of the streamgages in Oregon and Washington record major water quality parameters, and hundreds of sites in the area have discrete sampling for a wide range of water quality constituents. Still, numerous gaps exist in understanding the short- and long-term impacts of wildfire on hydrology, water chemistry, including pH and dissolved oxygen, mobilization of metals, aquatic ecosystems, and downstream drinking water treatment. Collective action to further collect, analyze, interpret, and publish the key data could help improve our understanding of post-wildfire water quality impacts in this and other increasingly wildfire-affected regions.

Forest harvesting can lead to mercury (Hg) mobilization from soils to aquatic habitats and promote the transformation of inorganic Hg to highly neurotoxic and bioaccumulative methyl-Hg (MeHg). Multiple past studies reveal broad variation of stream water MeHg and total Hg (THg) concentration responses to forest harvesting, which has confounded messaging to forest and resource managers. To advance beyond divergent and sometimes contradictory findings, we synthesized information for 23 previously studied catchments in North America and Fennoscandia and compiled a uniform set of soil, landscape, and harvesting properties to identify forest management, riparian, and hillslope factors that influence responses of stream water MeHg and THg concentrations. From this synthesis, we found catchments with high soil moisture and organic soil layers >100 cm to be at highest risk for disturbance-induced increases in MeHg formation after harvest but not necessarily affecting concentrations of MeHg in stream waters. Instead, the combination of MeHg formation in soils along with factors that affect mobilization with runoff to streams most influenced how forest harvest affects MeHg concentrations in stream waters.

The mobility and bioavailability of metal contaminants such as lead (Pb) and zinc (Zn) is impacted by their interactions with other sediment constituents such as iron (Fe), sulfur (S), and organic matter, which depend on sediment redox conditions. Understanding the role that water level fluctuations have on redox conditions and subsequent impacts on metal mobility is critical for predicting impacts of increased wetting and drying cycles resulting from climate-related changes or management actions. This study measured the sediment-porewater partitioning of Pb and Zn in the Coeur d'Alene River basin downstream of the Bunker Hill Superfund Site under both flooded and seasonally dry conditions. The results show that both time of year and hydrology are important when considering metal exposure risks in contaminated floodplains. For Pb, seasonal spring flooding appears to mobilize dissolved Pb in both seasonally inundated and permanently inundated areas due to increases in sediment-derived Pb that undergo desorption processes from suspended Fe and DOC. For Zn, oxygenation of floodplain sediments in the fall drives elevated dissolved Zn year-round due to limited ZnS precipitation. Wetting-drying cycles had a significant impact on Zn mobility, which could be exacerbated by climate-driven hydrological changes or floodplain management actions.

Ecosystems downstream of mercury (Hg) contaminated sites can be impacted by both localized releases as well as Hg deposited to the watershed from atmospheric transport. Identifying the source of Hg in water, sediment, and fish downstream of contaminated sites is important for determining the effectiveness of source-control remediation actions. This study uses measurements of Hg stable isotopes in soil, sediment, water, and fish to differentiate between Hg from an abandoned Hg mine from non-mine-related sources. The study site is located within the Willamette River watershed (Oregon, United States), which includes free-flowing river segments and a reservoir downstream of the mine. The concentrations of total-Hg (THg) in the reservoir fish were 4-fold higher than those further downstream (>90 km) from the mine site in free-flowing sections of the river. Mercury stable isotope fractionation analysis showed that the mine tailings (δ 202 Hg: −0.36‰ ± 0.03‰) had a distinctive isotopic composition compared to background soils (δ 202 Hg: −2.30‰ ± 0.25‰). Similar differences in isotopic composition were observed between stream water that flowed through the tailings (particulate bound δ 202 Hg: −0.58‰; dissolved: −0.91‰) versus a background stream (particle-bound δ 202 Hg: −2.36‰; dissolved: −2.09‰). Within the reservoir sediment, the Hg isotopic composition indicated that the proportion of the Hg related to mine-release increased with THg concentrations. However, in the fish samples the opposite trend was observed—the degree of mine-related Hg was lower in fish with the higher THg concentrations. While sediment concentrations clearly show the influence of the mine, the relationship in fish is more complicated due to differences in methylmercury (MeHg) formation and the foraging behavior of different fish species. The fish tissue δ 13 C and Δ 199 Hg values indicate that there is a higher influence of mine-sourced Hg in fish feeding in a more sediment-based food web and less so in planktonic and littoral-based food webs. Identifying the relative proportion of Hg from local contaminated site can help inform remediation decisions, especially when the relationship between total Hg concentrations and sources do not show similar covariation between abiotic and biotic media.

Mercury methylation frequently occurs at the active oxic/anoxic boundary between the sediment bed and water column of lakes and reservoirs. Previous studies suggest that the predominant mercury methylation zone moves to the water column during periods of stratification and that high potential methylation rates (Km) in sediment require oxygenated overlying water. However, simultaneous measurements of methylmercury (MeHg) produc-tion in both the sediment and water column remain limited. Understanding the relative importance of sediment versus water column methylation and the impact of seasonal stratification on these processes has important implications for managing MeHg production. This study measured Km and potential demethylation rates (Kdm) using stable isotope tracers of unfiltered inorganic mercury and MeHg in sediments and water of the littoral and profundal zones of a shallow branch of the Nacimiento Reservoir in California's central coastal range. Field sampling was conducted once during winter (well-mixed/oxygenated conditions) and once during late summer (thermally stratified/anoxic conditions). The results showed very high ambient MeHg concentrations in hypo-limnetic waters (up to 7.5 ng L-1; 79% MeHg/total Hg). During late summer, littoral sediments had higher Km (0.024 day -1) compared to profundal sediments (0.013 day -1). Anoxic water column Km were of similar magnitude to Km in the sediment (0.03 day -1). Following turnover, profundal sediment Km did not change significantly, but water column Km became insignificant. Summer and winter sediment Kdm were higher in profundal (2.35, 3.54 day -1, respectively) compared to the littoral sediments (0.52, 2.56 day -1, respectively). When modelled, Km in the water column could account for approximately 40% of the hypolimnetic MeHg. Our modelling results show that the remaining MeHg in the hypolimnion could originate from the profundal sedi-ment. While further study is needed, these results suggest that addressing methylation in the water column and profundal sediment are of equal importance to any remediation strategy.

Biochar can reduce lead (Pb) bioavailability to plants in metal-contaminated soil, but the ability of biochar to reduce the bioavailability of soil Pb to people and wildlife remains unknown. In this study, 17 biochars were evaluated as in situ amendments for three soils with distinct sources of Pb contamination (smelter emissions, ceramics waste, mining waste), hydrology (upland, well-drained soil vs submerged wetland soil), and biological receptors (human vs waterfowl). Biochars were made from blends of 30% manure (poultry litter or dairy manure) and 70% lignocellulosic material (wheat straw or grand fir shavings) and pyrolyzed at 300, 500, 700, and 900 °C. Soils were amended with 2% biochar (w/w) and incubated for 6 months. A suite of standard (e.g., EPA Method 1340) and experimental soil Pb bioaccessibility assays were used to assess the impact of the treatments. The results showed that biochar amendments to upland soils resulted in modest reductions in gastrointestinal Pb bioaccessibility (maximum reduction from 78 to 68% bioaccessibility as a percent of total, EPA Method 1340 at pH 2.5). In the wetland soil, sample redox status had a greater impact on Pb bioaccessibility than any amendment. Low-solubility Pb sulfides in this soil oxidized over the course of the study and no treatment was able to offset the increase in Pb bioaccessibility caused by this oxidation. The impact of redox status on Pb bioaccessibility was only evident when soil bioaccessibility assays were adapted to preserve sample redox status. This result highlights the importance of maintaining in situ redox conditions when processing/analyzing samples from low-oxygen environments and that soil remediation efforts should consider the role of redox conditions on Pb bioaccessibility.

Increased cell membrane permeability to sodium is proposed as the initial event leading to high blood pressure in susceptible subjects when sodium intake is increased. All cells, including circulating cells, would be affected, but a key role for endothelial cells in the pathophysiology of the diastolic blood pressure elevation is proposed. Involvement of capillary endothelium could increase capillary permeability to proteins, and thereby would contribute to the altered fluid distribution on the high sodium diet which has been observed. If movement of fluid into the interstitium raised interstitial fluid pressure, venous capacitance would fall and right atrial pressure would rise. Several mechanisms would cause vascular smooth muscle tone to increase. Altered fluid distribution correlates with the rise in diastolic blood pressure from reduced sodium to high sodium diet, but arteriolar constriction would reduce capillary flow so altered fluid distribution occurs first. Arteriolar constriction could serve as a negative feedback to the raised atrial filling pressure by reducing raised capillary flow, which would decrease both altered fluid distribution and interstitial fluid pressure rise. Consequently, diastolic blood pressure would be chronically raised in ‘sodium sensitive’ subjects taking increased amounts of sodium in the diet. The relationship of the findings to “essential” hypertension and to premorbid cardiovascular sequelae, and the key role of capillary endothelium in the development of “essential” hypertension is discussed.

Methylmercury (MeHg) is a highly toxic form of mercury that can bioaccumulate in fish tissue. Methylmercury is produced by anaerobic bacteria, many of which are also capable of MeHg degradation. In addition, demethylation in surface waters can occur via abiotic sunlight-mediated processes. The goal of the present study was to understand the relative importance of microbial Hg methylation/demethylation and abiotic photodemethylation that govern the mass of MeHg within an aquatic system. The study location was the Hells Canyon complex of 3 reservoirs on the Idaho-Oregon border, USA, that has fish consumption advisories as a result of elevated MeHg concentrations. Our study utilized stable isotope addition experiments to trace MeHg formation and degradation within the water column of the reservoirs to understand the relative importance of these processes on the mass of MeHg using the Water Quality Analysis Simulation Program. The results showed that rates of MeHg production and degradation within the water column were relatively low (<0.07 d-1 ) but sufficient to account for most of the MeHg observed with the system. Most MeHg production within the water column appeared to occur in the spring when much of the water column was in the processes of becoming anoxic. In the surface waters, rates of photodemethylation were relatively large (up to -0.25 d-1 ) but quickly decreased at depths >0.5 m below the surface. These results can be used to identify the relative importance of MeHg processes that can help guide reservoir management decisions. Environ Toxicol Chem 2021;40:1829-1839. © 2021 SETAC. This article has been contributed to by US Government employees and their work is in the public domain in the USA.

Thousands of abandoned mines throughout the western region of North America contain elevated total-mercury (THg) concentrations. Mercury is mobilized from these sites primarily due to erosion of particulate-bound Hg (THg-P). Organic matter-based soil amendments can promote vegetation growth on mine tailings, reducing erosion and subsequent loading of THg-P into downstream waterbodies. However, the introduction of a labile carbon source may stimulate microbial activity that can produce methylmercury (MeHg)-the more toxic and bioaccumulative form of Hg. Our objectives were to investigate how additions of different organic matter substrates impact Hg mobilization and methylation using a combination of field observations and controlled experiments. Field measurements of water, sediment, and porewater were collected downstream of the site and multi-year monitoring (and load calculations) were conducted at a downstream gaging station. MeHg production was assessed using stable isotope methylation assays and mesocosm experiments that were conducted using different types of organic carbon soil amendments mixed with materials from the mine site. The results showed that >80% of the THg mobilized from the mine was bound to particles and that >90% of the annual Hg loading occurred during the period of elevated discharge during spring snowmelt. Methylation rates varied between different types of soil amendments and were correlated with the components of excitation emission matrices (EEMs) associated with humic acid fractions of organic matter. The mesocosm experiments showed that under anoxic conditions carbon amendments to tailings could significantly increase porewater MeHg concentrations (up to 13 ± 3 ng/L). In addition, the carbon amendments significantly increased THg partitioning into porewater. Overall, these results indicate that soil amendment applications to reduce surface erosion at abandoned mine sites could be effective at reducing particulate Hg mobilization to downstream waterbodies; however, some types of carbon amendments can significantly increase Hg methylation as well as increase the mobilization of dissolved THg from the site.

Remediation of mercury (Hg) contaminated sites has long relied on traditional approaches, such as removal and containment/capping. Here we review contemporary practices in the assessment and remediation of industrial-scale Hg contaminated sites and discuss recent advances. Significant improvements have been made in site assessment, including the use of XRF to rapidly identify the spatial extent of contamination, Hg stable isotope fractionation to identify sources and transformation processes, and solid-phase characterization (XAFS) to evaluate Hg forms. The understanding of Hg bioavailability for methylation has been improved by methods such as sequential chemical extractions and porewater measurements, including the use of diffuse gradient in thin-film (DGT) samplers. These approaches have shown varying success in identifying bioavailable Hg fractions and further study and field applications are needed. The downstream accumulation of methylmercury (MeHg) in biota is a concern at many contaminated sites. Identifying the variables limiting/controlling MeHg production-such as bioavailable inorganic Hg, organic carbon, and/or terminal electron acceptors (e.g. sulfate, iron) is critical. Mercury can be released from contaminated sites to the air and water, both of which are influenced by meteorological and hydrological conditions. Mercury mobilized from contaminated sites is predominantly bound to particles, highly correlated with total sediment solids (TSS), and elevated during stormflow. Remediation techniques to address Hg contamination can include the removal or containment of Hg contaminated materials, the application of amendments to reduce mobility and bioavailability, landscape/waterbody manipulations to reduce MeHg production, and food web manipulations through stocking or extirpation to reduce MeHg accumulated in desired species. These approaches often rely on knowledge of the Hg forms/speciation at the site, and utilize physical, chemical, thermal and biological methods to achieve remediation goals. Overall, the complexity of Hg cycling allows many different opportunities to reduce/mitigate impacts, which creates flexibility in determining suitable and logistically feasible remedies.

The focus of this paper is to briefly discuss the major advances in scientific thinking regarding: a) processes governing the fate and transport of mercury in the environment; b) advances in measurement methods; and c) how these advances in knowledge fit in within the context of the Minamata Convention on Mercury. Details regarding the information summarized here can be found in the papers associated with this Virtual Special Issue of STOTEN.

We report on the continuous ambient measurements of total gaseous mercury (TGM) and several ancillary air quality parameters that were collected in Colorado Springs, CO. This urban area, which is located adjacent to the Front Range of the Rocky Mountains, is the second largest metropolitan area in Colorado and has a centrally located coal-fired power plant that installed mercury (Hg) emission controls the year prior to our study. There are few other Hg point sources within the city. Our results, which were obtained from a measurement site < 1 km from the power plant, show a distinct diel pattern in TGM, with peak concentrations occurring during the night (1.7 ± 0.3 ng m−3) and minimum concentrations mid-day (1.5 ± 0.2 ng m−3). The TGM concentrations were not correlated with wind originating from the direction of the plant or with sulfur dioxide (SO2) mixing ratios, and they were not elevated when the atmospheric mixing height was above the effective stack height. These findings suggest that the current Hg emissions from the CFPP did not significantly influence local TGM, and they are consistent with the facility’s relatively low reported annual emissions of 0.20 kg Hg per year. Instead, variability in the regional signal, diurnal meteorological conditions, and/or near-surface emission sources appears to more greatly influence TGM at this urban site.

Timber harvest has many effects on aquatic ecosystems, including changes in hydrological, biogeochemical, and ecological processes that can influence mercury (Hg) cycling. Although timber harvest's influence on aqueous Hg transformation and transport are well studied, the effects on Hg bioaccumulation are not. We evaluated Hg bioaccumulation, biomagnification, and food web structure in 10 paired catchments that were either clear-cut in their entirety, clear-cut except for an 8-m wide riparian buffer, or left unharvested. Average mercury concentrations in aquatic biota from clear-cut catchments were 50% higher than in reference catchments and 165% higher than in catchments with a riparian buffer. Mercury concentrations in aquatic invertebrates and salamanders were not correlated with aqueous THg or MeHg concentrations, but rather treatment effects appeared to correspond with differences in the utilization of terrestrial and aquatic basal resources in the stream food webs. Carbon and nitrogen isotope data suggest that a diminished shredder niche in the clear-cut catchments contributed to lower basal resource diversity compared with the reference of buffered treatments, and that elevated Hg concentrations in the clear-cut catchments reflect an increased reliance on aquatic resources in clear-cut catchments. In contrast, catchments with riparian buffers had higher basal resource diversity than the reference catchments, indicative of more balanced utilization of terrestrial and aquatic resources. Further, following timber harvest THg concentrations in riparian songbirds were elevated, suggesting an influence of timber harvest on Hg export to riparian food webs. These data, coupled with comparisons of individual feeding guilds, indicate that changes in organic matter sources and associated effects on stream food web structure are important mechanisms by which timber harvest modifies Hg bioaccumulation in headwater streams and riparian consumers.

Guest editors Heileen Hsu-Kim, Chris Eckley, and Noelle Selin introduce the Mercury Biogeochemistry, Exposure, and Impacts themed issue of Environmental Science: Processes & Impacts.

Mercury is a global pollutant released into the biosphere by varied human activities including coal combustion, mining, artisanal gold mining, cement production, and chemical production. Once released to air, land and water, the addition of carbon atoms to mercury by bacteria results in the production of methylmercury, the toxic form that bioaccumulates in aquatic and terrestrial food chains resulting in elevated exposure to humans and wildlife. Global recognition of the mercury contamination problem has resulted in the Minamata Convention on Mercury, which came into force in 2017. The treaty aims to protect human health and the environment from human-generated releases of mercury curtailing its movement and transformations in the biosphere. Coincident with the treaty's coming into force, the 13th International Conference of Mercury as a Global Pollutant (ICMGP-13) was held in Providence, Rhode Island USA. At ICMGP-13, cutting edge research was summarized and presented to address questions relating to global and regional sources and cycling of mercury, how that mercury is methylated, the effects of mercury exposure on humans and wildlife, and the science needed for successful implementation of the Minamata Convention. Human activities have the potential to enhance mercury methylation by remobilizing previously released mercury, and increasing methylation efficiency. This synthesis concluded that many of the most important factors influencing the fate and effects of mercury and its more toxic form, methylmercury, stem from environmental changes that are much broader in scope than mercury releases alone. Alterations of mercury cycling, methylmercury bioavailability and trophic transfer due to climate and land use changes remain critical uncertainties in effective implementation of the Minamata Convention. In the face of these uncertainties, important policy and management actions are needed over the short-term to support the control of mercury releases to land, water and air. These include adequate monitoring and communication on risk from exposure to various forms of inorganic mercury as well as methylmercury from fish and rice consumption. Successful management of global and local mercury pollution will require integration of mercury research and policy in a changing world.

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.

Land-use activities can alter hydrological and biogeochemical processes that can affect the fate, transformation, and transport of mercury (Hg). Previous studies in boreal forests have shown that forestry operations can have profound but variable effects on Hg export and methylmercury (MeHg) formation. The Pacific Northwest is an important timber producing region that receives large atmospheric Hg loads, but the impact of forest harvesting on Hg mobilization has not been directly studied and was the focus of our investigation. Stream discharge was measured continuously, and Hg and MeHg concentrations were measured monthly for 1.5 years following logging in three paired harvested and unharvested (control) catchments. There was no significant difference in particulate-bound Hg concentrations or loads in the harvested and unharvested catchments which may have resulted from forestry practices aimed at minimizing erosion. However, the harvested catchments had significantly higher discharge (32%), filtered Hg concentrations (28%), filtered Hg loads (80%), and dissolved organic carbon (DOC) loads (40%) compared to forested catchments. MeHg concentrations were low (mostly <0.05 ng L-1) in harvested, unharvested, and downstream samples due to well-drained/unsaturated soil conditions and steep slopes with high energy eroding stream channels that were not conducive to the development of anoxic conditions that support methylation. These results have important implications for the role forestry operations have in affecting catchment retention and export of Hg pollution.

Reservoirs typically have elevated fish mercury (Hg) levels compared to natural lakes and rivers. A unique feature of reservoirs is water-level management which can result in sediment exposure to the air. The objective of this study is to identify how reservoir water-level fluctuations impact Hg cycling, particularly the formation of the more toxic and bioaccumulative methylmercury (MeHg). Total-Hg (THg), MeHg, stable isotope methylation rates and several ancillary parameters were measured in reservoir sediments (including some in porewater and overlying water) that are seasonally and permanently inundated. The results showed that sediment and porewater MeHg concentrations were over 3-times higher in areas experiencing water-level fluctuations compared to permanently inundated sediments. Analysis of the data suggest that the enhanced breakdown of organic matter in sediments experiencing water-level fluctuations has a two-fold effect on stimulating Hg methylation: 1) it increases the partitioning of inorganic Hg from the solid phase into the porewater phase (lower log Kd values) where it is more bioavailable for methylation; and 2) it increases dissolved organic carbon (DOC) in the porewater which can stimulate the microbial community that can methylate Hg. Sulfate concentrations and cycling were enhanced in the seasonally inundated sediments and may have also contributed to increased MeHg production. Overall, our results suggest that reservoir management actions can have an impact on the sediment-porewater characteristics that affect MeHg production. Such findings are also relevant to natural water systems that experience wetting and drying cycles, such as floodplains and ombrotrophic wetlands.