Mercury Inputs Research Articles

Co-analysis of total suspended particles and discharge reveals the dynamic of mercury input into glacier meltwater runoff in the northern Tibetan Plateau

Climate warming has accelerated glacier melting, releasing legacy pollutants such as mercury (Hg) into aquatic ecosystems. While the relationship between Hg in glacier meltwater runoff, total suspended particles (TSP), and runoff discharges has been established, the underlying inter-relationships and governing factors remain poorly understood. To address this knowledge gap, we conducted a continuous fixed-point sampling at Laohugou No. 12 Glacier in the northern Tibetan Plateau from June to September 2019 spanning the entire glacier ablation season. Our study analyzed the variations of Hg partition in the meltwater runoff and conducted a comprehensive co-analysis of Hg with TSP and discharge to uncover the dominant factors of Hg input into meltwater runoff. The concentration of total Hg (THg) in the meltwater runoff ranged from 0.7 to 112.6 ng/L, with an average concentration of 26.6 ± 25.1 ng/L. Particulate Hg (PHg) was found to be the predominant partition, while dissolved Hg (DHg) exhibited a notable increase in June and September. THg concentration significantly correlated with TSP concentration (r = 0.94, P < 0.01), exceeding the correlation with discharge (r = 0.76, P < 0.01) during the entire ablation period. However, further examination during varying hydrological periods revealed differing associations among Hg speciation concentrations, TSP concentration, and discharge. During the rising limb of the hydrograph, THg (r = 0.86, P < 0.01) and PHg concentrations (r = 0.87, P < 0.01) exhibited a significant correlation with TSP concentration, primarily driven by TSP, implying that Hg availability determines the Hg input into meltwater runoff. Conversely, during the recession limb of the hydrograph, THg concentration was primarily influenced by discharge (r = 0.85, P < 0.01). PHg (r = 0.84, P < 0.01) and TSP (r = 0.97, P < 0.01) concentrations were strongly influenced by discharge, indicating that hydraulic action is the dominant factor affecting Hg input. Our study elucidated the impact of glacier hydrological processes on Hg transport, revealing the dominant factors of Hg input during different hydrological periods. This contributes to a deeper understanding of Hg input into meltwater runoff and improves predictions of Hg export through glacier melt in high mountain regions.

Dominant host phase of mercury within the sediments of the East China Sea inner shelf: Implications for mercury inputs

Mercury (Hg) concentrations normalized to their dominant hosts have been widely used to identify geological events such as massive volcanic eruptions. However, the modern Hg cycle has significantly changed, and the implications of host-normalized Hg concentrations for the Hg dynamics in contemporary coastal environments (e.g., sources, delivery mechanisms, and Hg fluxes) remain poorly understood. In this study, 66 surface sediment samples from the continental shelf of the East China Sea (ECS) were analyzed, and the total organic carbon (TOC), aluminum (Al), total sulfur (TS), and Hg concentrations were determined. Our results support that organic matter predominantly hosts Hg in these sediments. Factors such as the Hg source and abundances of organic fractions influence Hg distributions, with notable enrichment in the Changjiang River estuary and the inner shelf of the ECS, especially near the mud depocenter located off the Oujiang River estuary. The oxic to suboxic redox state and the lack of significant sulfide accumulation in surface sediments suggest that sulfides are not the primary Hg hosts. The Hg/TOC ratios, ranging from 3.0 to 169.6 (ppb/%), are particularly high in the Changjiang River estuary and exhibit an exponential correlation with the Hg accumulation rates (Hg-AR). These findings suggest that the host-normalized Hg concentration could serve as a valuable tool for assessing Hg dynamics where the accumulation rates are uncertain.

Exploring Drivers of Historic Mercury Trends in Beluga Whales Using an Ecosystem Modeling Approach.

While mercury occurs naturally in the environment, human activity has significantly disturbed its biogeochemical cycle. Inorganic mercury entering aquatic systems can be transformed into methylmercury, a strong neurotoxicant that builds up in organisms and affects ecosystem and public health. In the Arctic, top predators such as beluga whales, an ecologically and culturally significant species for many Inuit communities, can contain high concentrations of methylmercury. Historical mercury concentrations in beluga in the western Canadian Arctic's Beaufort Sea cannot be explained by mercury emission trends alone; in addition, they could potentially be driven by climate change impacts, such as rising temperatures and sea ice melt. These changes can affect mercury bioaccumulation through different pathways, including ecological and mercury transport processes. In this study, we explore key drivers of mercury bioaccumulation in the Beaufort Sea beluga population using Ecopath with Ecosim, an ecosystem modeling approach, and scenarios of environmental change informed by Western Science and Inuvialuit Knowledge. Comparing the effect of historical sea ice cover, sea surface temperature, and freshwater discharge time series, modeling suggests that the timing of historical increases and decreases in beluga methylmercury concentrations can be better explained by the resulting changes to ecosystem productivity rather than by those to mercury inputs and that all three environmental drivers could partially explain the decrease in mercury concentrations in beluga after the mid-1990s. This work highlights the value of multiple knowledge systems and exploratory modeling methods in understanding environmental change and contaminant cycling. Future work building on this research could inform climate change adaptation efforts and inform management decisions in the region.

Spatial Variation in Mercury Accumulation in Bottlenose Dolphins (Tursiops spp.) in Southeastern U.S.A.

Bottlenose dolphins (Tursiops spp.) inhabit bays, sounds, and estuaries (BSEs) throughout the southeast region of the U.S.A. and are sentinel species for human and ecosystem-level health. Dolphins are vulnerable to the bioaccumulation of contaminants through the coastal food chain because they are high-level predators. Currently, there is limited information on the spatial dynamics of mercury accumulation in these dolphins. Total mercury (THg) was measured in dolphin skin from multiple populations across the U.S. Southeast Atlantic and Gulf of Mexico coasts, and the influence of geographic origin, sex, and age class was investigated. Mercury varied significantly among sampling sites and was greatest in dolphins in St. Joseph Bay, Florida Everglades, and Choctawhatchee Bay (14,193 ng/g ± 2196 ng/g, 10,916 ng/g ± 1532 ng/g, and 7333 ng/g ± 1405 ng/g wet mass (wm), respectively) and lowest in dolphins in Charleston and Skidaway River Estuary (509 ng/g ± 32.1 ng/g and 530 ng/g ± 58.4 ng/g wm, respectively). Spatial mercury patterns were consistent regardless of sex or age class. Bottlenose dolphin mercury exposure can effectively represent regional trends and reflect large-scale atmospheric mercury input and local biogeochemical processes. As a sentinel species, the bottlenose dolphin data presented here can direct future studies to evaluate mercury exposure to human residents in St. Joseph Bay, Choctawhatchee Bay, and Florida Coastal Everglades, as well as additional sites with similar geographical, oceanographic, or anthropogenic parameters. These data may also inform state and federal authorities that establish fish consumption advisories to determine if residents in these locales are at heightened risk for mercury toxicity.

Temporal mercury dynamics throughout the rice cultivation season in the Ebro Delta (NE Spain): An integrative approach

During the last few decades, inputs of mercury (Hg) to the environment from anthropogenic sources have increased. The Ebro Delta is an important area of rice production in the Iberian Peninsula. Given the industrial activity and its legacy pollution along the Ebro river, residues containing Hg have been transported throughout the Ebro Delta ecosystems. Rice paddies are regarded as propitious environments for Hg methylation and its subsequent incorporation to plants and rice paddies' food webs. We have analyzed how Hg dynamics change throughout the rice cultivation season in different compartments from the paddies' ecosystems: soil, water, rice plants and fauna. Furthermore, we assessed the effect of different agricultural practices (ecological vs. conventional) associated to various flooding patterns (wet vs. mild alternating wet and dry) to the Hg levels in rice fields. Finally, we have estimated the proportion of methylmercury (MeHg) to total mercury in a subset of samples, as MeHg is the most bioaccumulable toxic form for humans and wildlife. Overall, we observed varying degrees of mercury concentration over the rice cultivation season in the different compartments. We found that different agricultural practices and flooding patterns did not influence the THg levels observed in water, soil or plants. However, Hg concentrations in fauna samples seemed to be affected by hydroperiod and we also observed evidence of Hg biomagnification along the rice fields’ aquatic food webs.

Large mercury release from the Greenland Ice Sheet invalidated.

The major input of mercury (Hg) to the Arctic is normally ascribed to long-range transport of anthropogenic Hg emissions. Recently, alarming concentrations of Hg in meltwater from the Greenland Ice Sheet (GrIS) were reported with bedrock as the proposed source. Reported Hg concentrations were 100 to 1000 times higher than in known freshwater systems of Greenland, calling for independent validation of the extraordinary concentrations and conclusions. Here, we present measurements of Hg at 21 glacial outlets in West Greenland showing that extreme Hg concentrations cannot be reproduced. In contrast, we find that meltwater from below the GrIS is very low in Hg, has minor implications for the global Hg budget, and pose only a very limited risk for local communities and the natural environment of Greenland.

Tree foliage as a net accumulator of highly toxic methylmercury

Tree canopies are known to elevate atmospheric inputs of both mercury (Hg) and methylmercury (MeHg). While foliar uptake of gaseous Hg is well documented, little is known regarding the temporal dynamics and origins of MeHg in tree foliage, which represents typically less than 1% of total Hg in foliage. In this work, we examined the foliar total Hg and MeHg content by following the growth of five individual trees of American Beech (Fagus grandifolia) for one growing season (April–November, 2017) in North Carolina, USA. We show that similar to other studies foliar Hg content increased almost linearly over time, with daily accumulation rates ranging from 0.123 to 0.161 ng/g/day. However, not all trees showed linear increases of foliar MeHg content along the growing season; we found that 2 out of 5 trees showed elevated foliar MeHg content at the initial phase of the growing season but their MeHg content declined through early summer. However, foliar MeHg content among all 5 trees showed eventual increases through the end of the growing season, proving that foliage is a net accumulator of MeHg while foliar gain of biomass did not “dilute” MeHg content.

Distribution and trends of mercury in aquatic and terrestrial biota of New York, USA: a synthesis of 50 years of research and monitoring.

Mercury (Hg) inputs have particularly impacted the northeastern United States due to its proximity to anthropogenic emissions sources and abundant habitats that efficiently convert inorganic Hg into methylmercury. Intensive research and monitoring efforts over the past 50 years in New York State, USA, have informed the assessment of the extent and impacts of Hg exposure on fishes and wildlife. By synthesizing Hg data statewide, this study quantified temporal trends of Hg exposure, spatiotemporal patterns of risk, the role that habitat and Hg deposition play in producing spatial patterns of Hg exposure in fish and other wildlife, and the effectiveness of current monitoring approaches in describing Hg trends. Most temporal trends were stable, but we found significant declines in Hg exposure over time in some long-sampled fish. The Adirondack Mountains and Long Island showed the greatest number of aquatic and terrestrial species with elevated Hg concentrations, reflecting an unequal distribution of exposure risk to fauna across the state. Persistent hotspots were detected for aquatic species in central New York and the Adirondack Mountains. Elevated Hg concentrations were associated with open water, forests, and rural, developed habitats for aquatic species, and open water and forested habitats for terrestrial species. Areas of consistently elevated Hg were found in areas driven by atmospheric and local Hg inputs, and habitat played a significant role in translating those inputs into biotic exposure. Continued long-term monitoring will be important in evaluating how these patterns continue to change in the face of changing land cover, climate, and Hg emissions.

Mercury Burial in Modern Sedimentary Systems of the East China Marginal Seas: The Role of Coastal Oceans in Global Mercury Cycling

AbstractCoastal oceans, the transition zones between terrestrial and oceanic systems, are susceptible to anthropogenic mercury (Hg) inputs and are regarded as critical dynamic interfaces of the global Hg cycle. However, the extent to which coastal oceans are accountable for sequestering Hg remains largely unknown owing to the lack of data on high‐resolution Hg accumulation in marine sediments. Synthesizing the results of this study (eight cores and 212 surface sediments) and the literature (three cores and 149 surface sediments), we provide a quantitative evaluation of the biogeochemical cycle of sedimentary Hg in the East China Marginal Seas (ECMS), including the response of the coastal marine sediments to anthropogenic disturbance as well as both human‐derived and natural Hg burial fluxes. We find a linear increase in Hg accumulation since the 1950s (2.0 ± 2.5% yr−1) and a decline in Hg accumulation between 2010 and 2016. Modern burial fluxes of total and anthropogenic Hg in the ECMS (covering ∼4.8 × 105 km2 of sea surface) were estimated to be 89.1 ± 48.3 and 35.9 ± 33.1 Mg yr−1, respectively. Using a compilation of 688 surface sediments and 131 sediment cores (819 samples in total) distributed globally in coastal oceans, we estimate that approximately 1,590 (range: 1,190–2,760) Mg yr−1 (Method 1) and 540 (range: 310–960) Mg yr−1 (Method 2) Hg are accumulated in coastal ocean regions. Our findings suggest that coastal oceans are likely the largest global marine sinks for Hg and play a dominant role in regulating the oceanic Hg cycle and budgets.

Mercury exposure in Antarctic seabirds: Assessing the influence of trophic position and migration patterns

Although naturally present in the environment, mercury (Hg) input is significantly amplified by anthropogenic activities on a global scale, leading to a growing concern about the recent increase in Hg levels observed in Antarctica. This study investigated total mercury (THg) concentrations in feathers and eggs of resident and migratory Antarctic seabirds. Stable isotope data (δ15N, δ13C, and δ34S) were employed to ascertain the key factors influencing the exposure of these species to Hg. We gathered feathers and eggs from three resident species - Adélie, Gentoo, and Chinstrap penguins, as well as five migratory species - Snowy Sheathbill, Antarctic Tern, Southern Giant Petrel, Kelp Gull, and South Polar Skua. These samples were collected from Admiralty Bay, King George Island, in the Antarctica Peninsula. For all species, THg concentrations were higher in feathers (mean ± SD: 2267 ± 2480 ng g−1 dw) than in eggs (906 ± 1461 ng g−1 dw). Species occupying higher trophic positions, such as the Southern Giant Petrel (5667 ± 1500 ng g−1 dw) and South Polar Skua (4216 ± 1101 ng. g−1 dw), exhibited higher THg levels in their feathers than those at lower positions, like Antarctic Tern (1254 ± 400 ng g−1 dw) and Chinstrap Penguin (910 ± 364 ng g−1 dw). The δ15N values, which serve as a proxy for the trophic position, significantly correlated with THg concentrations. These findings reveal that trophic position influences THg concentrations in Antarctic seabirds. Migration did not appear to significantly affect the exposure of seabirds to THg, contrary to initial expectations. This research highlights the importance of evaluating the impacts of THg contamination on the Antarctic ecosystem by considering a variety of species. This multi-species approach offers critical insights into the factors that may potentially influence the exposure of these species to contaminants.

Ornithogenic mercury input to soils of Admiralty Bay, King George Island, Antarctica

Ornithogenic mercury input to soils of Admiralty Bay, King George Island, Antarctica

Comparing ecosystem gaseous elemental mercury fluxes over a deciduous and coniferous forest

Sources of neurotoxic mercury in forests are dominated by atmospheric gaseous elemental mercury (GEM) deposition, but a dearth of direct GEM exchange measurements causes major uncertainties about processes that determine GEM sinks. Here we present three years of forest-level GEM deposition measurements in a coniferous forest and a deciduous forest in northeastern USA, along with flux partitioning into canopy and forest floor contributions. Annual GEM deposition is 13.4 ± 0.80 μg m−2 (coniferous forest) and 25.1 ± 2.4 μg m−2 (deciduous forest) dominating mercury inputs (62 and 76% of total deposition). GEM uptake dominates in daytime during active vegetation periods and correlates with CO2 assimilation, attributable to plant stomatal uptake of mercury. Non-stomatal GEM deposition occurs in the coniferous canopy during nights and to the forest floor in the deciduous forest and accounts for 24 and 39% of GEM deposition, respectively. Our study shows that GEM deposition includes various pathways and is highly ecosystem-specific, which complicates global constraints of terrestrial GEM sinks.

An examination of the factors influencing the bioaccumulation of methylmercury at the base of the estuarine food web

Estuarine systems have received ongoing mercury (Hg) inputs from both point sources and regional contamination and have high legacy Hg in sediments. This is an environmental concern given that coastal seafood is an important vector for human exposure to methylmercury (MeHg). The base of the food chain represents the most important trophic steps for MeHg bioaccumulation. The magnitude of the uptake by phytoplankton, and their consumers, is influenced by many factors, in addition to sediment and water MeHg concentrations, that impact MeHg assimilation into phytoplankton and the trophic transfer to higher trophic levels, both benthic and pelagic. For forage fish, such as mummichogs (Fundulus heteroclitus), abiotic and biotic (bioenergetic) factors can influence their MeHg content, and diet is also important as they feed both on benthic and pelagic prey. Given that the importance of sediment MeHg versus pelagic MeHg sources has been debated, we updated a phytoplankton bioaccumulation model, and coupled this with a bioaccumulation model for MeHg concentration in mummichog tissue to examine the controlling factors for sites, from Maine to Maryland, USA, ranging widely in their Hg concentrations and other variables. The study highlighted the importance of DOC in modulating uptake into the pelagic food web, but also demonstrated the importance of diet in controlling mummichog MeHg. Finally, the relative importance of MeHg source - sediment or water column – was correlated with the level of Hg contamination. Sediment-derived MeHg was a more important source for highly Hg contaminated systems. As water column and sediment MeHg are not strongly correlated for the studied ecosystems, their importance as a source of MeHg to mummichogs varies with location. The study highlights the differences across ecosystems in MeHg bioaccumulation pathways, and that uptake into phytoplankton is an important variable controlling forage fish concentration.

Mercury Pollution History in Tropical and Subtropical American Lakes: Multiple Impacts and the Possible Relationship with Climate Change.

Sediment cores obtained from 11 tropical and subtropical American lakes revealed that local human activities significantly increased mercury (Hg) inputs and pollution levels. Remote lakes also have been contaminated by anthropogenic Hg through atmospheric depositions. Long-term sediment-core profiles revealed an approximately 3-fold increase in Hg fluxes to sediments from c. 1850 to 2000. Generalized additive models indicate that c. 3-fold increases in Hg fluxes also occurred since 2000 in the remote sites, while Hg emissions from anthropogenic sources have remained relatively stable. The tropical and subtropical Americas are vulnerable to extreme weather events. Air temperatures in this region have shown a marked increase since the 1990s, and extreme weather events arising from climate change have increased. When comparing Hg fluxes to recent (1950-2016) climatic changes, results show marked increases in Hg fluxes to sediments during dry periods. The Standardized Precipitation-Evapotranspiration Index (SPEI) time series indicate a tendency toward more extreme drier conditions across the study region since the mid-1990s, suggesting that instabilities in catchment surfaces caused by climate change are responsible for the elevated Hg flux rates. Drier conditions since c. 2000 appear to be promoting Hg fluxes from catchments to lakes, a process that will likely be exacerbated under future climate-change scenarios.

Terrestrial rather than volcanic mercury inputs to the Yangtze Platform (South China) during the Ordovician-Silurian transition

The Hg proxy has been used to infer a close relationship between volcanism and the ‘Big Five’ Phanerozoic mass extinctions. However, because of conflicting interpretations of Hg data, this relationship remains in debate for the Late Ordovician mass extinction (LOME). In this study, three sections (Datianba, Shuanghe and YY1), located in shallow to deep shelf settings, were chosen for investigation of the Hg cycle on the Yangtze Platform during the Ordovician-Silurian transition (OST). Our results show that sulfur-normalized Hg concentrations (Hg/TS, TS: total sulfur) are the best proxy for assessing Hg anomalies in these sections due to Hg being hosted mainly by sulfide minerals. The Hg/TS profiles of the three study sections exhibit no enhanced Hg loading of a potential volcanic origin. Differing Al-Hg relationships among the study sections imply different Hg sources, with dominantly terrigenous Hg at Datianba and hydrogenous (seawater-derived) Hg at Shuanghe and YY1. This inference is supported by contrasting near-zero to weakly negative Δ199Hg values at Datianba versus positive Δ199Hg values at Shuanghe. These findings demonstrate the influence of terrigenously sourced Hg on Upper Ordovician sediments of the Yangtze Platform, and, in conjunction with the non-correlatability of Hg anomalies between the study sections and their lack of a stratigraphic relationship to bentonites, they do not support a relationship between the LOME and large igneous province (LIP) or arc volcanism in the South China region during the OST.

Screening of Mercury pollution sources to European inland waters using high resolution earth surface data

Mercury pollution is a cause of high concern for European freshwaters. In this study, we use modelled atmospheric deposition and novel high-resolution water cover and impervious urban areas data to quantify the input of Mercury to European rivers and lakes. This information, combined with estimates of releases from industrial installations and urban wastewater and from soils, yields an overall European budget of water Mercury. Compared to previous estimates, the calculation highlights that direct deposition to permanent and temporary inland water surfaces is a dominant source of pollution. We also show that an important source is the washout of impervious urban surfaces, while releases from soil and industrial and urban wastewater play a lesser, albeit sizable role. The contribution of wastewater to Mercury releases is expected to decrease over time because of more stringent regulations on Mercury use. The analysis confirms that reducing atmospheric deposition (hence air releases) of Mercury remains the single key action to control pollution. However, we show that control of urban runoff discharges to water bodies may be the most effective water management measure in order to reduce Mercury input to coastal and in-land water bodies.

Record of Middle Jurassic wildfire and its incidental mercury emissions in northern Qaidam Basin, China: Evidence from the inertinite and mercury anomalies in coal

Inertinite in coals contains important information regarding the palaeo-wildfire history and can provide insights into its triggers and relationship with the evolution of local ecosystems. However, such information in the Middle Jurassic coal is often overlooked, and the impacts of incidental mercury emission from wildfires on the mercury enrichment in coal are also underestimation. In this study, the organic petrology, geochemistry and palynology of coal seams from the coal-bearing member of Shimengou Formation in northern Qaidam Basin (NQB) were investigated. Results show that these coal seams generally contain abundant records of palaeo-wildfire: inertinite and combustion-derived polycyclic aromatic hydrocarbons (PAHs). The high consistency of these two evidences confirms the existence of widespread wildfires during the late Middle Jurassic (Bathonian) in NQB. These widespread wildfires also indicate a high level of atmospheric oxygen concentration during this period. The overall low inertinite reflectance (avg. 1.27%) and low content of coronene in coal seams indicate that these wildfires were dominated by ground and surface fire with some small-scale crown fires. These frequent wildfires under the overall humid climate are attributed to the sufficient atmospheric oxygen, fuel and intermittent dry season. The co-occurrence of wildfires records and mercury anomaly in coal seams suggests that incidental mercury emissions from wildfires enhanced mercury input in the peatlands, which is the direct trigger for mercury anomaly in the coal from the Shimengou Formation in NQB. This study not only revealed the characteristics and causes of the widespread wildfires during the late Middle Jurassic in NQB, but also provides a new insight into the abnormal enrichment of mercury in coal.

Arctic Ocean’s wintertime mercury concentrations limited by seasonal loss on the shelf

High biota mercury levels are persisting in the Arctic, threatening ecosystem and human health. The Arctic Ocean receives large pulsed mercury inputs from rivers and the atmosphere. Yet the fate of those inputs and possible seasonal variability of mercury in the Arctic Ocean remain uncertain. Until now, seawater observations were possible only during summer and fall. Here we report polar night mercury seawater observations on a gradient from the shelf into the Arctic Ocean. We observed lower and less variable total mercury concentrations during the polar night (winter, 0.46 ± 0.07 pmol l−1) compared with summer (0.63 ± 0.19 pmol l−1) and no substantial changes in methylmercury concentrations (summer, 0.11 ± 0.03 pmol l−1 and winter, 0.12 ± 0.04 pmol l−1). Seasonal changes were estimated by calculating the difference in the integrated mercury pools. We estimate losses of inorganic mercury of 208 ± 41 pmol m−2 d−1 on the shelf driven by seasonal particle scavenging. Persistent methylmercury concentrations (−1 ± 16 pmol m−2 d−1) are probably driven by a lower affinity for particles and the presence of gaseous species. Our results update the current understanding of Arctic mercury cycling and require budgets and models to be reevaluated with a seasonal aspect.

Are There Longitudinal Effects of Forest Harvesting on Carbon Quality and Flow and Methylmercury Bioaccumulation in Primary Consumers of Temperate Stream Networks?

Forest harvesting affects dissolved organic matter (DOM) and aqueous mercury inputs as well as the food web structure in small-headwater streams, but how these upstream changes manifest downstream is unclear. To address this uncertainty, we examined DOM quality, autochthony in the caddisfly Hydropsychidae (using δ2 H), and methylmercury (MeHg) concentrations in stream water and the caddisfly along a longitudinal gradient (first- to fourth-order streams, subcatchments of 50-1900 ha) in paired partially harvested and reference catchments in central Ontario, Canada. Although measures of DOM quality (specific ultraviolet absorbance at 254 nm 2.20-11.62) and autochthony in caddisflies (4.9%-34.0%) varied among sites, no upstream-to-downstream differences in these measures were observed between the paired harvested and reference catchments. In contrast, MeHg levels in stream water (0.06-0.35 ng/L) and caddisflies(29.7-192 µg/kg dry wt) were significantly higher in the upstream sites but not the farthest downstream sites in the harvested catchments compared to the reference catchments. This suggests that while current mitigation measures used by forestry companies did not prevent elevated MeHg in water and invertebrates at smaller spatial scales (subcatchments of 50-400 ha), these upstream impacts did not manifest at larger spatial scales (subcatchments of 800-1900 ha). The present study advances our understanding of spatially cumulative impacts within harvested catchments, which is critical to help forest managers maintain healthy forest streams and their provisioning of aquatic ecosystem services. Environ Toxicol Chem 2022;41:1490-1507. © 2022 SETAC.

Source Apportionment of Speciated Mercury in Chinese Rice Grain Using a High-Resolution Model.

Rice grain consumption is a primary pathway of human mercury exposure. To trace the source of rice grain mercury in China, we developed a rice paddy mercury transport and transformation model with a grid resolution of 1 km × 1 km by using the unit cell mass conservation method. The simulated total mercury (THg) and methylmercury (MeHg) concentrations in Chinese rice grain ranged from 0.08 to 243.6 and 0.03 to 238.6 μg/kg, respectively, in 2017. Approximately, 81.3% of the national average rice grain THg concentration was due to atmospheric mercury deposition. However, soil heterogeneity, especially the variation in soil mercury, led to the wide rice grain THg distribution across grids. Approximately, 64.8% of the national average rice grain MeHg concentration was due to soil mercury. In situ methylation was the main pathway via which the rice grain MeHg concentration was increased. The coupled impact of high mercury input and methylation potential led to extremely high rice grain MeHg in partial grids among Guizhou province and junctions with surrounding provinces. The spatial variation in soil organic matter significantly impacted the methylation potential among grids, especially in Northeast China. Based on the high-resolution rice grain THg concentration, we identified 0.72% of grids as heavily polluted THg grids (rice grain THg > 20 μg/kg). These grids mainly corresponded to areas in which the human activities of nonferrous metal smelting, cement clinker production, and mercury and other metal mining were conducted. Thus, we recommended measures that are targeted at the control of heavy pollution of rice grain by THg according to the pollution sources. In addition, we observed a wide spatial variation range of MeHg to THg ratios not only in China but also in other regions of the world, which highlights the potential risk of rice intake.