Distinct dynamics in mountain watersheds: Exploring mercury and microplastic pollution-Unraveling the influence of atmospheric deposition, human activities, and hydrology.

The intensification of human activities all around the globe has led to the spread of micropollutants in high-mountain freshwater environments. We therefore aimed to assess the geospatial distribution and determine the potential sources of (total-) mercury (THg) and microplastics (MPs) in mountain freshwater ecosystems. To do so, we analyzed THg and MP concentrations in brown trout, biofilm, and sediments from lotic and lentic ecosystems in the Pyrenees - all subjected to different types of human pressure. Additionally, we assessed the potential impacts of these pollutants on fish, and explored the bioindication capacity of brown trout (Salmo trutta fario) and biofilm regarding THg and MP pollution. For the first time, we measured concentrations of MPs trapped in the matrix of freshwater biofilm. Our results suggest that THg in the Pyrenees might be explained by both legacy (regional) and distant sources, in combination with environmental characteristics such as the presence of peatlands or streamwater physicochemistry, while MPs in fish are linked to recent local pollution sources such as single-use plastics. In contrast, MPs in biofilm matrix and sediments indicate a combination of distant (i.e., atmospheric deposition) and recent local pollution sources. Moreover, hydrodynamics and plastic density likely control MP distribution in rivers. Based on Fulton's condition factor, we also found that higher THg concentrations caused a negative impact on fish health (K < 1), while no impact of MPs could be seen. Therefore, we suggest that brown trout and biofilm can serve as bioindicators of atmospheric deposition of THg in high-altitude lakes and that biofilm is a reliable bioindicator to assess MP pollution in remote environments. Brown trout may also act as a bioindicator of MP pollution, but only efficiently in more polluted areas.

Over a decade of atmospheric mercury monitoring at Amsterdam Island in the French Southern and Antarctic Lands.

The Minamata Convention, a global and legally binding treaty that entered into force in 2017, aims to protect human health and the environment from harmful mercury (Hg) effects by reducing anthropogenic Hg emissions and environmental levels. The Conference of the Parties is to periodically evaluate the Convention's effectiveness, starting in 2023, using existing monitoring data and observed trends. Monitoring atmospheric Hg levels has been proposed as a key indicator. However, data gaps exist, especially in the Southern Hemisphere. Here, we present over a decade of atmospheric Hg monitoring data at Amsterdam Island (37.80°S, 77.55°E), in the remote southern Indian Ocean. Datasets include gaseous elemental and oxidised Hg species ambient air concentrations from either active/continuous or passive/discrete acquisition methods, and annual total Hg wet deposition fluxes. These datasets are made available to the community to support policy-making and further scientific advancements.

Global change effects on biogeochemical mercury cycling.

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.

Trace mercury migration and human exposure in typical mercury-emission areas by compound-specific stable isotope analysis.

Anthropogenic mercury (Hg) emissions have increased significantly since the Industrial Revolution, resulting in severe health impacts to humans. The consumptions of fish and rice were primary human methylmercury (MeHg) exposure pathways in Asia. However, the lifecycle from anthropogenic Hg emissions to human MeHg exposure is not fully understood. In this study, a recently developed approach, termed MeHg Compound-Specific Isotope Analysis (CSIA), was employed to track lifecycle of Hg in four typical Hg-emission areas. Distinct Δ199Hg of MeHg and inorganic Hg (IHg) were observed among rice, fish and hair. The Δ199Hg of MeHg averaged at 0.07 ± 0.15 ‰, 0.80 ± 0.55 ‰ and 0.43 ± 0.29 ‰ in rice, fish and hair, respectively, while those of IHg averaged at - 0.08 ± 0.24 ‰, 0.85 ± 0.43 ‰ and - 0.28 ± 0.68 ‰. In paddy ecosystem, Δ199Hg of MeHg in rice showed slightly positive shifts (∼0.2 ‰) from those of IHg, and comparable Δ199Hg of IHg between rice grain and raw/processed materials (coal, Hg ore, gold ore and sphalerite) were observed. Simultaneously, it was proved that IHg in fish muscle was partially derived from in vivo demethylation of MeHg. By a binary model, we estimated the relative contributions of rice consumption to human MeHg exposure to be 84 ± 14 %, 58 ± 26 %, 52 ± 20 % and 34 ± 15 % on average in Hg mining area, gold mining area, zinc smelting area and coal-fired power plant area, respectively, and positive shifts of δ202HgMeHg from fish/rice to human hair occurred during human metabolic processes. Therefore, the CSIA approach can be an effective tool for tracking Hg biogeochemical cycle and human exposure, from which new scientific knowledge can be generated to support Hg pollution control policies and to protect human health.

PET plastics as a Trojan horse for radionuclides.

Mismanaged plastic waste interacts with secondary environmental pollutants, potentially aggravating their impact on ecosystems and human health. Here we characterized the natural and artificial radionuclides in polyethylene terephthalate (PET) bottles collected from the industrial littoral discharge of a phosphate fertilizer plant. The activity concentrations in littered bottles ranged from 0.47 (208Tl) to 12.70 Bq·kg-1 (226Ra), with a mean value of 5.30 Bq·kg-1. All the human health risk assessment indices (annual intake, annual effective dose, and excess lifetime cancer risk) estimated for radionuclides associated with ingestion and inhalation of microplastics were below international safety limits. Our results demonstrated that PET can be loaded with natural and artificial radionuclides, and potentially act as a carrier to transfer radionuclides to humans, posing a new potential health risk. Increased use, mismanagement and fragmentation of plastic waste, and continued interaction of plastic waste with radioelements may lead to enhanced radiation exposure in the future.

Mercury isotope evidence for Arctic summertime re-emission of mercury from the cryosphere.

During Arctic springtime, halogen radicals oxidize atmospheric elemental mercury (Hg0), which deposits to the cryosphere. This is followed by a summertime atmospheric Hg0 peak that is thought to result mostly from terrestrial Hg inputs to the Arctic Ocean, followed by photoreduction and emission to air. The large terrestrial Hg contribution to the Arctic Ocean and global atmosphere has raised concern over the potential release of permafrost Hg, via rivers and coastal erosion, with Arctic warming. Here we investigate Hg isotope variability of Arctic atmospheric, marine, and terrestrial Hg. We observe highly characteristic Hg isotope signatures during the summertime peak that reflect re-emission of Hg deposited to the cryosphere during spring. Air mass back trajectories support a cryospheric Hg emission source but no major terrestrial source. This implies that terrestrial Hg inputs to the Arctic Ocean remain in the marine ecosystem, without substantial loss to the global atmosphere, but with possible effects on food webs.

Mercury stable isotopes suggest reduced foraging depth in oxygen minimum zones for blue sharks.

Oxygen minimum zones (OMZs) are currently expanding across the global ocean due to climate change, leading to a compression of usable habitat for several marine species. Mercury stable isotope compositions provide a spatially and temporally integrated view of marine predator foraging habitat and its variability with environmental conditions. Here, we analyzed mercury isotopes in blue sharks Prionace glauca from normoxic waters in the northeastern Atlantic and from the world's largest and shallowest OMZ, located in the northeastern Pacific (NEP). Blue sharks from the NEP OMZ area showed higher Δ199Hg values compared to sharks from the northeastern Atlantic, indicating a reduction in foraging depth of approximately 200 m. Our study suggests for the first time that blue shark feeding depth is altered by expanding OMZs and illustrates the use of mercury isotopes to assess the impacts of ocean deoxygenation on the vertical foraging habitat of pelagic predators.

Mediterranean Mercury Assessment 2022: An Updated Budget, Health Consequences, and Research Perspectives.

Mercury (Hg) and especially its methylated species (MeHg) are toxic chemicals that contaminate humans via the consumption of seafood. The most recent UNEP Global Mercury Assessment stressed that Mediterranean populations have higher Hg levels than people elsewhere in Europe. The present Critical Review updates current knowledge on the sources, biogeochemical cycling, and mass balance of Hg in the Mediterranean and identifies perspectives for future research especially in the context of global change. Concentrations of Hg in the Western Mediterranean average 0.86 ± 0.27 pmol L-1 in the upper water layer and 1.02 ± 0.12 pmol L-1 in intermediate and deep waters. In the Eastern Mediterranean, Hg measurements are in the same range but are too few to determine any consistent oceanographical pattern. The Mediterranean waters have a high methylation capacity, with MeHg representing up to 86% of the total Hg, and constitute a source of MeHg for the adjacent North Atlantic Ocean. The highest MeHg concentrations are associated with low oxygen water masses, suggesting a microbiological control on Hg methylation, consistent with the identification of hgcA-like genes in Mediterranean waters. MeHg concentrations are twice as high in the waters of the Western Basin compared to the ultra-oligotrophic Eastern Basin waters. This difference appears to be transferred through the food webs and the Hg content in predators to be ultimately controlled by MeHg concentrations of the waters of their foraging zones. Many Mediterranean top-predatory fish still exceed European Union regulatory Hg thresholds. This emphasizes the necessity of monitoring the exposure of Mediterranean populations, to formulate adequate mitigation strategies and recommendations, without advising against seafood consumption. This review also points out other insufficiencies of knowledge of Hg cycling in the Mediterranean Sea, including temporal variations in air-sea exchange, hydrothermal and cold seep inputs, point sources, submarine groundwater discharge, and exchanges between margins and the open sea. Future assessment of global change impacts under the Minamata Convention Hg policy requires long-term observations and dedicated high-resolution Earth System Models for the Mediterranean region.

Foraging plasticity diversifies mercury exposure sources and bioaccumulation patterns in the world's largest predatory fish.

Large marine predators exhibit high concentrations of mercury (Hg) as neurotoxic methylmercury, and the potential impacts of global change on Hg contamination in these species remain highly debated. Current contaminant model predictions do not account for intraspecific variability in Hg exposure and may fail to reflect the diversity of future Hg levels among conspecific populations or individuals, especially for top predators displaying a wide range of ecological traits. Here, we used Hg isotopic compositions to show that Hg exposure sources varied significantly between and within three populations of white sharks (Carcharodon carcharias) with contrasting ecology: the north-eastern Pacific, eastern Australasian, and south-western Australasian populations. Through Δ200Hg signatures in shark tissues, we found that atmospheric Hg deposition pathways to the marine environment differed between coastal and offshore habitats. Discrepancies in δ202Hg and Δ199Hg signatures among white sharks provided evidence for intraspecific exposure to distinct sources of marine methylmercury, attributed to population and ontogenetic shifts in foraging habitat and prey composition. We finally observed a strong divergence in Hg accumulation rates between populations, leading to three times higher Hg concentrations in large Australasian sharks compared to north-eastern Pacific sharks, and likely due to different trophic strategies adopted by adult sharks across populations. This study illustrates the variety of Hg exposure sources and bioaccumulation patterns that can be found within a single species and suggests that intraspecific variability needs to be considered when assessing future trajectories of Hg levels in marine predators.

Evidence that Pacific tuna mercury levels are driven by marine methylmercury production and anthropogenic inputs.

Pacific Ocean tuna is among the most-consumed seafood products but contains relatively high levels of the neurotoxin methylmercury. Limited observations suggest tuna mercury levels vary in space and time, yet the drivers are not well understood. Here, we map mercury concentrations in skipjack tuna across the Pacific Ocean and build generalized additive models to quantify the anthropogenic, ecological, and biogeochemical drivers. Skipjack mercury levels display a fivefold spatial gradient, with maximum concentrations in the northwest near Asia, intermediate values in the east, and the lowest levels in the west, southwest, and central Pacific. Large spatial differences can be explained by the depth of the seawater methylmercury peak near low-oxygen zones, leading to enhanced tuna mercury concentrations in regions where oxygen depletion is shallow. Despite this natural biogeochemical control, the mercury hotspot in tuna caught near Asia is explained by elevated atmospheric mercury concentrations and/or mercury river inputs to the coastal shelf. While we cannot ignore the legacy mercury contribution from other regions to the Pacific Ocean (e.g., North America and Europe), our results suggest that recent anthropogenic mercury release, which is currently largest in Asia, contributes directly to present-day human mercury exposure.

ENSO Climate Forcing of the Marine Mercury Cycle in the Peruvian Upwelling Zone Does Not Affect Methylmercury Levels of Marine Avian Top Predators.

Climate change is expected to affect marine mercury (Hg) biogeochemistry and biomagnification. Recent modeling work suggested that ocean warming increases methylmercury (MeHg) levels in fish. Here, we studied the influence of El Niño Southern Oscillations (ENSO) on Hg concentrations and stable isotopes in time series of seabird blood from the Peruvian upwelling and oxygen minimum zone. Between 2009 and 2016, La Niña (2011) and El Niño conditions (2015-2016) were accompanied by sea surface temperature anomalies up to 3 °C, oxycline depth change (20-100 m), and strong primary production gradients. Seabird Hg levels were stable and did not co-vary significantly with oceanographic parameters, nor with anchovy biomass, the primary dietary source to seabirds (90%). In contrast, seabird Δ199Hg, proxy for marine photochemical MeHg breakdown, and δ15N showed strong interannual variability (up to 0.8 and 3‰, respectively) and sharply decreased during El Niño. We suggest that lower Δ199Hg during El Niño represents reduced MeHg photodegradation due to the deepening of the oxycline. This process was balanced by equally reduced Hg methylation due to reduced productivity, carbon export, and remineralization. The non-dependence of seabird MeHg levels on strong ENSO variability suggests that marine predator MeHg levels may not be as sensitive to climate change as is currently thought.

Mercury stable isotopes constrain atmospheric sources to the ocean.

Human exposure to toxic mercury (Hg) is dominated by the consumption of seafood1,2. Earth system models suggest that Hg in marine ecosystems is supplied by atmospheric wet and dry Hg(II) deposition, with a three times smaller contribution from gaseous Hg(0) uptake3,4. Observations of marine Hg(II) deposition and Hg(0) gas exchange are sparse, however5, leaving the suggested importance of Hg(II) deposition6 ill-constrained. Here we present the first Hg stable isotope measurements of total Hg (tHg) in surface and deep Atlantic and Mediterranean seawater and use them to quantify atmospheric Hg deposition pathways. We observe overall similar tHg isotope compositions, with median Δ200Hg signatures of 0.02‰, lying in between atmospheric Hg(0) and Hg(II) deposition end-members. We use a Δ200Hg isotope mass balance to estimate that seawater tHg can be explained by the mixing of 42% (median; interquartile range, 24-50%) atmospheric Hg(II) gross deposition and 58% (50-76%) Hg(0) gross uptake. We measure and compile additional, global marine Hg isotope data including particulate Hg, sediments and biota and observe a latitudinal Δ200Hg gradient that indicates larger ocean Hg(0) uptake at high latitudes. Our findings suggest that global atmospheric Hg(0) uptake by the oceans is equal to Hg(II) deposition, which has implications for our understanding of atmospheric Hg dispersal and marine ecosystem recovery.

Compound-Specific Stable Isotope Analysis Provides New Insights for Tracking Human Monomethylmercury Exposure Sources.

Monomethylmercury (MMHg) exposure can induce adverse neurodevelopmental effects in humans and is a global environmental health concern. Human exposure to MMHg occurs predominately through the consumption of fishery foods and rice in Asia, but it is challenging to quantify these two exposure sources. Here, we innovatively utilized MMHg compound-specific stable isotope analyses (MMHg-CSIA) of the hair to quantify the human MMHg sources in coastal and inland areas, where fishery foods and rice are routinely consumed. Our data showed that the fishery foods and rice end members had distinct Δ199HgMMHg values in both coastal and inland areas. The Δ199HgMMHg values of the human hair were comparable to those of fishery foods but not those of rice. Positive shifts in the δ202HgMMHg values of the hair from diet were observed in the study areas. Additionally, significant differences in δ202Hg versus Δ199Hg were detected between MMHg and inorganic Hg (IHg) in the human hair but not in fishery foods and rice. A binary mixing model was developed to estimate the human MMHg exposures from fishery foods and rice using Δ199HgMMHg data. The model results suggested that human MMHg exposures were dominated (>80%) by fishery food consumption and were less affected by rice consumption in both the coastal and inland areas. This study demonstrated that the MMHg-CSIA method can provide unique information for tracking human MMHg exposure sources by excluding the deviations from dietary surveys, individual MMHg absorption/demethylation efficiencies, and the confounding effects of IHg.

Mass-Independent Fractionation of Even and Odd Mercury Isotopes during Atmospheric Mercury Redox Reactions.

Mass-independent fractionation (MIF) of stable even mass number mercury (Hg) isotopes is observed in rainfall and gaseous elemental Hg0 globally and is used to quantify atmospheric Hg deposition pathways. The chemical reaction and underlying even-Hg MIF mechanism are unknown however and speculated to be caused by Hg photo-oxidation on aerosols at the tropopause. Here, we investigate the Hg isotope composition of free tropospheric Hg0 and oxidized HgII forms at the high-altitude Pic du Midi Observatory. We find that gaseous oxidized Hg has positive Δ199Hg, Δ201Hg, and Δ200Hg and negative Δ204Hg signatures, similar to rainfall Hg, and we document rainfall Hg Δ196Hg to be near zero. Cloud water and rainfall Hg show an enhanced odd-Hg MIF of 0.3‰ compared to gaseous oxidized HgII, potentially indicating the occurrence of in-cloud aqueous HgII photoreduction. Diurnal MIF observations of free tropospheric Hg0 show how net Hg0 oxidation in high-altitude air masses leads to opposite even- and odd-MIF in Hg0 and oxidized HgII. We speculate that even-Hg MIF takes place by a molecular magnetic isotope effect during HgII photoreduction on aerosols that involves magnetic halogen nuclei. A Δ200Hg mass balance suggests that global Hg deposition pathways in models are likely biased toward HgII deposition. We propose that Hg cycling models could accommodate the Hg-isotope constraints on emission and deposition fluxes.

Hg concentrations and stable isotope variations in tropical fish species of a gold-mining-impacted watershed in French Guiana.

The aim of the study was to determine if gold-mining activities could impact the mercury (Hg) concentrations and isotopic signatures in freshwater fish consumed by riparian people in French Guiana. Total Hg, MeHg concentrations, and Hg stable isotopes ratios were analyzed in fish muscles from different species belonging to three feeding patterns (herbivorous, periphytophagous, and piscivorous). We compared tributaries impacted by gold-mining activities (Camopi, CR) with a pristine area upstream (Trois-Sauts, TS), along the Oyapock River. We measured δ15N and δ 13C to examine whether Hg patterns are due to differences in trophic level. Differences in δ 15N and δ 13C values between both studied sites were only observed for periphytophagous fish, due to difference of CN baselines, with enriched values at TS. Total Hg concentrations and Hg stable isotope signatures showed that Hg accumulated in fish from both areas has undergone different biogeochemical processes. Δ199Hg variation in fish (-0.5 to 0.2‰) was higher than the ecosystem baseline defined by a Δ199Hg of -0.66‰ in sediments, and suggested limited aqueous photochemical MeHg degradation. Photochemistry-corrected δ202Hg in fish was 0.7‰ higher than the baseline, consistent with biophysical and chemical isotope fractionation in the aquatic environment. While THg concentrations in periphytophagous fish were higher in the gold-mining area, disturbed by inputs of suspended particles, than in TS, the ensemble of Hg isotope shifts in fish is affected by the difference of biotic (methylation/demethylation) and abiotic (photochemistry) processes between both areas and did therefore not allow to resolve the contribution of gold-mining-related liquid Hg(0) in fish tissues. Mercury isotopes of MeHg in fish and lower trophic level organisms can be complementary to light stable isotope tracers.

Concentrations and stable isotopes of mercury in sharks of the Galapagos Marine Reserve: Human health concerns and feeding patterns.

The human ingestion of mercury (Hg) from sea food is of big concern worldwide due to adverse health effects, and more specifically if shark consumption constitutes a regular part of the human diet. In this study, the total mercury (THg) concentration in muscle tissue were determined in six sympatric shark species found in a fishing vessel seized in the Galapagos Marine Reserve in 2017. The THg concentrations in shark muscle samples (n = 73) varied from 0.73 mg kg-1 in bigeye thresher sharks (Alopias superciliosus) to 8.29 mg kg-1 in silky sharks (Carcharhinus falciformis). A typical pattern of Hg bioaccumulation was observed for all shark species, with significant correlation between THg concentration and shark size for bigeye thresher sharks, pelagic thresher sharks (Alopias pelagicus) and silky sharks. Regarding human health concerns, the THg mean concentration exceeded the maximum weekly intake fish serving in all the studied species. Mass-Dependent Fractionation (MDF, δ202Hg values) and Mass-Independent Fractionation (MIF, Δ199Hg values) of Hg in whitetip sharks (Carcharhinus longimanus) and silky sharks, ranged from 0.70‰ to 1.08‰, and from 1.97‰ to 2.89‰, respectively. These high values suggest that both species are feeding in the epipelagic zone (i.e. upper 200 m of the water column). While, blue sharks (Prionace glauca), scalloped hammerhead sharks (Shyrna lewini) and thresher sharks were characterized by lower Δ199Hg and δ202Hg values, indicating that these species may focus their foraging behavior on prey of mesopelagic zone (i.e. between 200 and 1000 m depth). In conclusion, the determination of THg concentration provides straight-forward evidence of the human health risks associated with shark consumption, while mercury isotopic compositions constitute a powerful tool to trace the foraging strategies of these marine predators. CAPSULE: A double approach combining Hg concentrations with stable isotopes ratios allowed to assess ontogeny in common shark species in the area of the Galapagos Marine Reserve and the human health risks concern associated to their consumption.

The Twilight Zone as a Major Foraging Habitat and Mercury Source for the Great White Shark.

The twilight zone contains the largest biomass of the world's ocean. Identifying its role in the trophic supply and contaminant exposure of marine megafauna constitutes a critical challenge in the context of global change. The white shark (Carcharodon carcharias) is a threatened species with some of the highest concentrations of neurotoxin methylmercury (MeHg) among marine top predators. Large white sharks migrate seasonally from coastal habitats, where they primarily forage on pinnipeds, to oceanic offshore habitats. Tagging studies suggest that while offshore, white sharks may forage at depth on mesopelagic species, yet no biochemical evidence exists. Here, we used mercury isotopic composition to assess the dietary origin of MeHg contamination in white sharks from the Northeast Pacific Ocean. We estimated that a minimum of 72% of the MeHg accumulated by white sharks originates from the consumption of mesopelagic prey, while a maximum of 25% derives from pinnipeds. In addition to highlighting the potential of mercury isotopes to decipher the complex ecological cycle of marine predators, our study provides evidence that the twilight zone constitutes a crucial foraging habitat for these large predators, which had been suspected for over a decade. Climate change is predicted to expand the production of mesopelagic MeHg and modify the mesopelagic biomass globally. Considering the pivotal role of the twilight zone is therefore essential to better predict both MeHg exposure and trophic supply to white sharks, and effectively protect these key vulnerable predators.

Photochemistry of oxidized Hg(I) and Hg(II) species suggests missing mercury oxidation in the troposphere.

Mercury (Hg), a global contaminant, is emitted mainly in its elemental form Hg0 to the atmosphere where it is oxidized to reactive HgII compounds, which efficiently deposit to surface ecosystems. Therefore, the chemical cycling between the elemental and oxidized Hg forms in the atmosphere determines the scale and geographical pattern of global Hg deposition. Recent advances in the photochemistry of gas-phase oxidized HgI and HgII species postulate their photodissociation back to Hg0 as a crucial step in the atmospheric Hg redox cycle. However, the significance of these photodissociation mechanisms on atmospheric Hg chemistry, lifetime, and surface deposition remains uncertain. Here we implement a comprehensive and quantitative mechanism of the photochemical and thermal atmospheric reactions between Hg0, HgI, and HgII species in a global model and evaluate the results against atmospheric Hg observations. We find that the photochemistry of HgI and HgII leads to insufficient Hg oxidation globally. The combined efficient photoreduction of HgI and HgII to Hg0 competes with thermal oxidation of Hg0, resulting in a large model overestimation of 99% of measured Hg0 and underestimation of 51% of oxidized Hg and ∼66% of HgII wet deposition. This in turn leads to a significant increase in the calculated global atmospheric Hg lifetime of 20 mo, which is unrealistically longer than the 3-6-mo range based on observed atmospheric Hg variability. These results show that the HgI and HgII photoreduction processes largely offset the efficiency of bromine-initiated Hg0 oxidation and reveal missing Hg oxidation processes in the troposphere.

Methylmercury produced in upper oceans accumulates in deep Mariana Trench fauna.

Monomethylmercury (MMHg) is a potent toxin that bioaccumulates and magnifies in marine food webs. Recent studies show abundant methylated Hg in deep oceans (>1000 m), yet its origin remains uncertain. Here we measured Hg isotope compositions in fauna and surface sediments from the Mariana Trench. The trench fauna at 7000-11000 m depth all have substantially positive mass-independent fractionation of odd Hg isotopes (odd-MIF), which can be generated only in the photic zone via MMHg photo-degradation. Given the identical odd-MIF in trench fauna and North Pacific upper ocean (<1000 m) biota MMHg, we suggest that the accumulated Hg in trench fauna originates exclusively from MMHg produced in upper oceans, which penetrates to depth by sorption to sinking particles. Our findings reveal little in-situ MMHg production in deep oceans and imply that anthropogenic Hg released at the Earth's surface is much more pervasive across deep oceans than was previously thought.