Hg Deposition Research Articles

Mercury evidence of Emeishan volcanism driving the mid-Capitanian (Middle Permian) extinction

The mid-Capitanian (Middle Permian) extinction has been widely attributed to the eruption of the Emeishan large igneous province. Here, we investigate the nature and timing of this link by determining Hg concentrations and isotopic compositions of limestones from the Xiongjiachang section of southwestern China, where Emeishan basalts directly overlie sediments recording the mid-Capitanian extinction horizon. Results show an initial Hg-enrichment interval ∼2.2 m below the mid-Capitanian extinction horizon. Positive Δ199Hg values in the Hg-enrichment interval suggest enhanced volcanic Hg influx into the ocean via atmospheric Hg(II) deposition. The late stage of the mid-Capitanian extinction interval has lower Δ199Hg values, which indicates enhanced input of terrestrial Hg due to ecosystem collapse and soil erosion. The results of this study provide evidence that the Emeishan large igneous province eruption occurred earlier than the mid-Capitanian extinction, and establish a more reasonable temporal link between Emeishan large igneous province volcanism and the mid-Capitanian extinction.

Terrestrial input and biological processes drive varying mineral/organic matrix-related mercury sequestration and deposition in the East Siberian Arctic Shelf

Thawing Arctic permafrost is releasing massive amounts of terrestrial mercury (Hg) into the Arctic shelf, which is expected to form a Hg sink in sediments. Here we analyzed the coupling roles of terrestrial input and biological processes in varying mineral/organic matrix-related Hg sequestration and deposition on the East Siberian Arctic shelf (ESAS), using Pearson and partial correlation analysis. Results show that the occurrence of Hg in the Laptev Sea under the Lena River-dominated input exhibits strong correlations with the organic carbon (OC) content and sediment specific surface area. This indicates that the prolonged riverine loading processes facilitate Hg sequestration by organic/mineral matrices and these land-derived mineral-OC-Hg complexes remain stable during cross-shelf transportation. By contrast, the comparative samples with coastal erosion-dominated Hg input in the western East Siberian Sea shows limited Hg complexation, primarily due to the absence of regulation by riverine processes and/or the high sedimentation rates. The correlations between Hg and OC source proxies (δ13C and lignin) indicate that these matrix-free Hg could be more readily sequestrated by the marine OC, which facilitates its deposition via the biological pump. While unexpectedly low Hg abundance in the Chukchi Sea may indicate that the effective biological scavenging of Hg sequestration could be constrained by insufficient terrestrial Hg input. Our findings of the matrix-related Hg sequestration by mineral and/or OC association in this study may shed light on the biogeochemical cycle of Hg in the Arctic aquatic regime, which could reduce the methylmercury formation in water column, and the methylation within sediments needs further exploration.

Atmospheric Mercury Concentrations and Isotopic Compositions Impacted by Typical Anthropogenic Mercury Emissions Sources.

Coal-fired power plants (CFPPs) and cement plants (CPs) are important anthropogenic mercury (Hg) emission sources. Mercury speciation profiles in flue gas are different among these sources, leading to significant variations in local atmospheric Hg deposition. To quantify the impacts of Hg emissions from CFPPs and CPs on local-scale atmospheric Hg deposition, this study determined concentrations and isotopes of ambient gaseous elemental mercury (GEM), particulate-bound mercury (PBM), and precipitation total Hg (THg) at multiple locations with different distances away from a CFPP and a CP. Higher concentrations of GEM and precipitation THg in the CFPP area in summer were caused by higher Hg emission from the CFPP, resulting from higher electricity demand. Higher concentrations of GEM, PBM, and precipitation THg in the CP area in winter compared to those in summer were related to the higher output of cement. Atmospheric Hg concentration peaked near the CFPP and CP and decreased with distance from the plants. Elevated GEM concentration in the CFPP area was due to flue gas Hg0 emissions, and high PBM and precipitation Hg concentrations in the CP area were attributed to divalent Hg emissions. It was estimated that Hg emissions from the CFPP contributed 58.3 ± 20.9 and 52.3 ± 25.9% to local GEM and PBM, respectively, and those from the CP contributed 47.0 ± 16.7 and 60.0 ± 25.9% to local GEM and PBM, respectively. This study demonstrates that speciated Hg from anthropogenic emissions posed distinct impacts on the local atmospheric Hg cycle, indicating that Hg speciation profiles from these sources should be considered for evaluating the effectiveness of emission reduction policies. This study also highlights the Hg isotope as a useful tool for monitoring environmental Hg emissions.

Unexpectedly high wet mercury deposition observed in the Yarlung Tsangpo Grand canyon

Situated in the south edge of the Tibetan Plateau, the Himalayas is expected to receive direct anthropogenic Hg perturbations from South Asia, yet the measurements of atmospheric Hg deposition in the Himalayan region remain scarce. Here we report wet Hg deposition measured in the Yarlung Tsangpo Grand Canyon of the Eastern Himalayas, which is the deepest and longest canyon on earth. The precipitation Hg concentration (56.3 ng L−1) and wet Hg deposition flux (84.7 μg m−2 yr−1) from the Motuo station were observed among the highest ever reported for the Tibetan Plateau. Together with analysis of principal component suggesting Hg was mainly clustered with anthropogenic ions and backward trajectories indicating 88.8% of air masses came from South Asia, our results show that transboudary pollution influences from South Asia could be largely responsible for the unexpectedly high levels of wet Hg deposition. Moreover, the wet Hg flux measurements (84.7 μg m−2 yr−1) are found an order of magnitude (∼13 times) higher than the GEOS-Chem estimates (6.8 μg m−2 yr−1), most likely due to the underestimation of transboundary Hg pollution influence by this model. Our study has important implications for better understanding Hg dynamics and verifying atmospheric Hg models in the Tibetan Plateau and Himalayas region.

Repeated pulses of volcanism drove the end-Permian terrestrial crisis in northwest China

The Permo-Triassic mass extinction was linked to catastrophic environmental changes and large igneous province (LIP) volcanism. In addition to the widespread marine losses, the Permo–Triassic event was the most severe terrestrial ecological crisis in Earth’s history and the only known mass extinction among insects, but the cause of extinction on land remains unclear. In this study, high-resolution Hg concentration records and multiple-archive S-isotope analyses of sediments from the Junggar Basin (China) provide evidence of repeated pulses of volcanic-S (acid rain) and increased Hg loading culminating in a crisis of terrestrial biota in the Junggar Basin coeval with the interval of LIP emplacement. Minor S-isotope analyses are, however, inconsistent with total ozone layer collapse. Our data suggest that LIP volcanism repeatedly stressed end-Permian terrestrial environments in the ~300 kyr preceding the marine extinction locally via S-driven acidification and deposition of Hg, and globally via pulsed addition of CO2.

Historical co-enrichment, source attribution, and risk assessment of critical nutrients and heavy metal/metalloids in lake sediments: insights from Chaohu Lake, China.

In Chinese freshwater lakes, eutrophication often coincides with heavy metal/metalloids (HM/Ms) pollution, yet the coevolution of critical nutrients (P, S, Se) and HM/Ms (Cd, Hg, etc.) remains understudied. To address this gap, we conducted a sedimentary chemistry analysis on a 30cm-deep core, dating back approximately 200years, retrieved from Chaohu Lake, China. The age-depth model revealed a gradual increase in deposition rates over time. Notably, the concentrations and enrichment factors (EFs) of most target elements surged in the uppermost ~ 15cm layer, covering the period from 1953 to 2013, while both the concentrations and EFs in deeper layers remained relatively stable, except for Hg. This trend indicates a significant co-enrichment and near-synchronous increase in the levels and EFs of both nutrients and HM/Ms in the upper sediment layers since the mid-twentieth century. Anthropogenic factors were identified as the primary drivers of the enrichment of P, Se, Cd, Hg, Zn, and Te in the upper core, with their contributions also showing a coupled evolutionary trend over time. Conversely, geological activities governed the enrichment of elements in the lower half of the core. The gradual accumulation of anthropogenic Hg between the - 30 to - 15cm layers might be attributed to global Hg deposition resulting from the industrial revolution. The ecological risk index (RI) associated with HM/Ms loading has escalated rapidly over the past 50years, with Cd and Hg posing the greatest threats. Furthermore, the PMF model was applied to specifically quantify source contributions of these elements in the core, with anthropogenic and geogenic factors accounting for ~ 60 and ~ 40%, respectively. A good correlation (r2 = 0.87, p < 0.01) between the PMF and Ti-normalized method was observed, indicating their feasibility and cross-validation in source apportionment. Finally, we highlighted environment impact and health implications of the co-enrichment of nutrients and HM/Ms. This knowledge is crucial for developing strategies to protect freshwater ecosystems from the combined impacts of eutrophication and HM/Ms pollution, thereby promoting water environment and human health.

Cambrian mercury mineralization event in South China: Insights from U-Pb dating of hydrothermal dolomite in the large Chatian Hg district

The genesis of many giant mercury (Hg) deposits/belts is widely debated largely because of a lack of reliable ore-forming age constraints. The LA-ICP-MS/MS dolomite U-Pb were employed to date the large Chatian Hg district in Xiangxi-Qiandong Hg belt of South China. The mineralization of this district can be divided into three stages: an initial Pyrite-Quartz stage before mercury deposition, a main Cinnabar-Sphalerite-Dolomite (Dol I) stage, and a subsequent Dolomite vein (Dol II) stage after ore formation. Three Dol I samples from the Chashula and Touponao Hg deposits were chosen for U-Pb dating, yielding ages of 509.8 ± 7.4 Ma, 509.4 ± 4.7 Ma and 507.4 ± 4.0 Ma respectively, indicating the mineralization occurred in the Cambrian Miaolingian, concurrent with or shortly after the deposition of the host-rock. These ages correspond with the emplacement periods of two Large Igneous Provinces (LIP) (the Pinghe silicic SLIP and the Kalkarindji LIP) in northeastern Gondwana, as well as the mantle-derived rocks in the study region. Combined with previous mercury isotopic data, our study proposes that the large-scale Hg mineralization in the area most likely resulted from the mantle-derived fluids, which would have directly contributed a significant amount of Hg for ore formation. Furthermore, the close timeframe between the Cambrian Series 2-Miaolingian trilobite extinction events and Hg mineralization in South China, may suggests a potential direct connection between the widespread mercury release and mineralization and the Cambrian Series 2-Miaolingian trilobite crisis in the region.

Electrochemical quartz crystal microbalance study of underpotential deposition of mercury on iridium metal and iridium oxide

AbstractTo evaluate the properties of an Ir‐based catalyst (IrOx), which is the anode in polymer electrolyte membrane‐type water electrolysis, a new method for estimating the electrochemical surface area (ECSA) is required. ECSA evaluation using the underpotential deposition of mercury (Hg‐UPD) can be applied to metals and oxides. However, research regarding Hg‐UPD is needed because several Hg(II)/Hg(I) redox reactions occur simultaneously, and direct evidence of Hg‐UPD on IrOx has not been reported. We previously confirmed the Hg‐UPD phenomenon on Ir polycrystalline films using the electrochemical quartz crystal microbalance (EQCM) method. However, measurements on IrOx electrodes were not performed. In this study, Ir and IrOx electrodes are prepared by the sputtering method, and their Hg deposition behavior observed by EQCM. We quantitatively confirm Hg‐UPD on Ir metal surfaces and provide new evidence of Hg‐UPD on the IrOx surface. These results contribute to establishing the ECSA evaluation of various Ir‐based catalysts.

Mercury stocks in discontinuous permafrost and their mobilization by river migration in the Yukon River Basin

Abstract Rapid warming in the Arctic threatens to destabilize mercury (Hg) deposits contained within soils in permafrost regions. Yet current estimates of the amount of Hg in permafrost vary by ~4 times. Moreover, how Hg will be released to the environment as permafrost thaws remains poorly known, despite threats to water quality, human health, and the environment. Here we present new measurements of total mercury (THg) contents in discontinuous permafrost in the Yukon River Basin in Alaska. We collected riverbank and floodplain sediments from exposed banks and bars near the villages of Huslia and Beaver. Median THg contents were 49+13/-21 ng THg g sediment−1 and 39 +16 /-18 ng THg g sediment−1 for Huslia and Beaver, respectively (uncertainties as 15th and 85th percentiles). Corresponding THg:organic carbon ratios were 5.4+2 /-2.4 Gg THg Pg C-1 and 4.2+2.4 /-2.9 Gg THg Pg C-1. To constrain floodplain THg stocks, we combined measured THg contents with floodplain stratigraphy. Trends of THg increasing with smaller sediment size and calculated stocks in the upper 1 m and 3 m are similar to those suggested for this region by prior pan-Arctic studies. We combined THg stocks and river migration rates derived from remote sensing to estimate particulate THg erosional and depositional fluxes as river channels migrate across the floodplain. Results show similar fluxes within uncertainty into the river from erosion at both sites (95 +12 /-47 kg THg yr-1 and 26 +154/-13 kg THg yr-1 at Huslia and Beaver, respectively), but very different fluxes out of the river via deposition in aggrading bars (60 +40/-29 kg THg yr-1 and 10+5.3/-1.7 kg THg yr-1). Thus, a significant amount of THg is liberated from permafrost during bank erosion, while a variable but generally lesser portion is subsequently redeposited by migrating rivers.

Mercury deposition in central China from the Last Glacial Maximum to the early Holocene recorded in an accurately-dated stalagmite

Characterization of transport pathways and depositional changes in Mercury (Hg) and their connection to climatic and environmental changes on various time scales are crucial for better understanding the anthropogenic impacts on the global Hg cycle in the Anthropocene epoch. In this study, we examined Hg variations recorded in a stalagmite from central China, covering the period from 25.5 to 10.9 thousand years ago. Our data show a marked increase in Hg concentrations during the late Last Glacial Maximum, which coincided with the period of highest dust deposition on the Chinese Loess Plateau. Hg concentrations were lower during Heinrich events 1 and 2 and the Younger Dryas but higher during the Bølling-Allerød and the early Holocene. We suggest that regional dust load, which enhances atmospheric dry deposition of Hg, is the primary factor influencing Hg deposition in central China on glacial-interglacial timescales. On millennial-to-centennial timescales, climate also plays a significant role. Warmer and wetter conditions increase vegetation, litterfall, and soil/rock weathering, which in turn boost mineral dissolution and soil erosion in the vadose zone. These processes collectively result in higher Hg concentrations in the stalagmite.

Transport characteristics of heavy metals in the soil-atmosphere-wheat system in farming areas and development of multiple linear regression predictive model

Heavy metal accumulation in agricultural products has become a major concern. Previous studies have focused on the transport of heavy metals from the soil and their accumulation in crops. However, recent studies revealed that wheat leaves, ears, and awns can also transport and accumulate heavy metals. Wheat grains can be influenced by two sources of heavy metals: soil contamination and atmospheric deposition. To comprehend the transport characteristics of heavy metals in soil, atmospheric deposition, and wheat, 37 samples each for wheat rhizosphere soil, wheat roots, stems, leaves, and grains were collected. Fifteen samples of atmospheric dry deposition and atmospheric wet deposition were collected from Linshu County (northern area), China. Based on the test data, the characteristics of heavy metals and their distribution in the study area were analyzed. Migration patterns of heavy metals in crops from different sources were investigated using Pearson correlation and redundancy analysis. Finally, a predictive model for heavy metals in wheat grains was developed using multiple linear regression analysis. Significant disparities in the distribution of heavy metals existed among wheat roots, stems, leaves, and grains. The coefficient of variation of heavy metals in atmospheric deposition was relatively high, indicating discernible spatial patterns influenced by human activities. Notably, a positive correlation was observed between the concentration of heavy metals in wheat grains and atmospheric deposition of Hg, Cd, and Pb. Conversely, Zn and Ni levels in wheat grains were significantly negatively associated with soil Zn, Ni, pH, and OM content. The contribution of heavy metal elements from different sources varied in their impact on the grain's heavy metal content. Specifically, atmospheric deposition was the primary source of Hg and Pb in wheat grains, while Cd, Ni, Cu, and Zn were predominantly derived from soil. Using a multiple linear regression model, we could accurately predict Hg, Pb, Cd, Ni, Zn, and As concentrations in crop grains. This model can facilitate quantitative evaluation of ecological risk of heavy metals accumulation in crops in the study area.

Low mercury risks in paddy soils across the Pakistan

Mercury (Hg) is a globally distributed heavy metal. Here, we study Hg concentration and isotopic composition to understand the status of Hg pollution and its sources in Pakistan's paddy soil. The collected paddy soils (n = 500) across the country have an average THg concentration of 22.30 ± 21.74 ng/g. This low mean concentration suggests Hg pollution in Pakistan was not as severe as previously thought. Meanwhile, samples collected near brick kilns and industrial areas were significantly higher in THg than others, suggesting the influence of Hg emitted from point sources in certain areas. Soil physicochemical properties showed typical characteristic of mineral soils due to the study area's arid to semi-arid climate. Hg stable isotopes analysis, depicted mean Δ199Hg of −0.05 ± 0.12‰ and mean δ202Hg −0.45 ± 0.35‰, respectively, for contaminated sites, depicting Hg was primarily sourced from coal combustion by local anthropogenic sources. While uncontaminated sites show mean Δ199Hg of 0.15 ± 0.08‰, mean Δ200Hg of 0.06 ± 0.07‰ and mean δ202Hg of −0.32 ± 0.28‰, implying long-range transboundry Hg transport through wet Hg(II) deposition as a dominant Hg source. This study fills a significant knowledge gap regarding the Hg pollution status in Pakistan and suggests that the Hg risk in Pakistan paddies is generally low.

Key factors influencing Hg levels and trends in unperturbed oligotrophic temperate and boreal lakes

Mercury (Hg) is a toxic metal that presents a major risk to ecosystems, biota, human health, and remains a priority concern. In temperate and boreal lakes Hg and methylmercury (MMHg) are expected to vary as a function of atmospheric Hg deposition, lake water chemistry, catchment characteristics and climate variables. The aim of this study was to quantify Hg and MMHg in unperturbed oligotrophic lakes and to identify the factors controlling their distribution. We first hypothesized that lake Hg (and MMHg to lesser extent) spatial variations are linked to atmospheric deposition, catchment characteristics, and terrestrial exportation of dissolved organic carbon (DOC). We secondly examined if lake Hg concentrations have followed the decrease in atmospheric Hg emission observed between the mid-1990s to the end-2010s. We found that overall, atmospheric Hg has little impact on lake Hg and MMHg concentrations, which are both primarily influenced by DOC input originating from the forest catchment. The relationship between DOC and Hg differed between the spring and the fall, with a Hg-to-DOC ratio twice as high in spring. This seems related to snowmelt input of Hg (with a relatively reduced input of DOC) or the internal lake build-up of Hg during the ice-covered period. Of the 10 lakes intensively visited over a 20-year period, only 3 showed significant lake Hg decreases despite significant negative trends in atmospheric Hg concentrations, suggesting a lag between atmospheric and surface water temporal trends. Overall, terrestrial catchments retain around 80% of atmospheric Hg implying that large Hg pools have been built up in soils in the last decades. As such, the reduction of atmospheric Hg alone will not necessarily result in Hg decreases in lakes, since the Hg concentrations may be modulated by DOC export trends and catchment characteristics. This stresses the need to improve our understanding of the processes governing Hg transfers from catchments into lakes.

Quantifying the impact of anthropogenic emissions and aquatic environmental impacts on sedimentary mercury variations in a typical urban river

In urban and industrial regions, sedimentary mercury (Hg) serves as the crucial indicator for Hg pollution, posing potential risks to ecology and human health. The physicochemical processes of Hg in aquatic environments are influenced by various factors such as anthropogenic emissions and aquatic environmental impacts, making it challenging to quantify the drivers of total mercury (THg) variations. Here, we analyzed the spatiotemporal variations, quantified driving factors, and assessed accumulation risks of sedimentary THg from the mainstream of a typical urban river (Haihe River). THg in the urban region (37−3237 ng g−1) was significantly higher (t-test, p < 0.01) than in suburban (71−2317 ng g−1) and developing regions (156−916 ng g−1). The sedimentary THg in suburban and developing regions increased from 2003 to 2018, indicating the elevated atmospheric deposition of Hg. Together with the temperature, grain size of sediments, total organic carbon (TOC), the pH and salinity of water, 40 components of parent and substituted polycyclic aromatic hydrocarbons (PAHs) were first introduced to quantify the driver of sedimentary THg based on generalized additive model. Results showed that anthropogenic emissions, including three PAHs components (31%) and TOC (63%), accounted for 94% of sedimentary THg variations. The aquatic environmental impacts accounted for 5% of sedimentary THg variations. The geo-accumulation index of THg indicated moderate to heavy accumulation in the urban region. This study demonstrates that homologous pollutants such as PAHs can be used to trace sources and variations of Hg pollution, supporting their co-regulation as international conventions regulate pollutants.

Quarter century of mercury litterfall at a coniferous forest responding to climate change, Central Europe.

This work evaluated the 25-year-long trends (1994-2018) in mercury (Hg) concentrations and fluxes in spruce litterfall at a forest research plot Načetín (NAC) recovering from acidic deposition in the Ore Mountains, Czech Republic. The mean litterfall Hg deposition averaged 51 ± 18µgm-2year-1, which has been the highest litterfall Hg deposition reported up to date on the European continent. In contrast, the wet deposition (2017-2019) was an order of magnitude lower averaging at 2.5 ± 1.5µgm-2year-1. All the spruce litterfall components bark, twigs, needles, cones, and a mixture of unidentified fragments had elevated mean Hg concentrations relative to background sites averaging 256 ± 77, 234 ± 62, 119 ± 23, 95 ± 14, and 44 ± 15µg kg-1, respectively. Elevated litterfall Hg deposition and concentrations were attributed to the nearby local Hg emission source-coal-fired power plants. Temporally, the decrease of Czech Hg emissions since the 1990s was reflected by the decreasing trend of Hg concentrations in litterfall bark, cones, and twigs, while in needles and other material, Hg increased but insignificantly. Total litterfall ratios of Hg/C, Hg/N, and Hg/S were lower than those in soil O horizons averaging at 0.23 ± 0.04, 9.5 ± 2.0, and 170 ± 37μgg-1, respectively. Since the beginning of monitoring, total litterfall Hg/C exhibited no trend, Hg/N decreased, and Hg/S increased. The litterfall biomass deposition averaging at 469 ± 176gm-2year-1 increased through time resulting in an increased Hg litterfall deposition at NAC by 1.1µgm-2year-1 despite the decreases in Czech Hg emissions. Peaks of annual litterfall Hg deposition up to 96µgm-2year-1 at NAC during the 25years of monitoring resulted from weather extremes such as rime-snow accumulation, wind gusts, droughts, and insect infestation, which all significantly affected the annual biomass deposition. Based on our observations, further increases in biomass and litterfall Hg deposition rates can be expected due to the onset of bark beetle infestation and the increasing number of droughts caused by climate change.

Projecting Global Mercury Emissions and Deposition Under the Shared Socioeconomic Pathways

AbstractMercury (Hg) is a naturally occurring element that has been greatly enriched in the environment by human activities like mining and fossil fuel combustion. Despite commonalities in some carbon dioxide (CO2) and Hg emission sources, the implications of long‐range climate scenarios for anthropogenic Hg emissions have yet to be explored. Here, we present comprehensive projections of anthropogenic Hg emissions extending to the year 2300 and evaluate impacts on global atmospheric Hg deposition. Projections are based on four Shared Socioeconomic Pathways (SSPs) ranging from sustainable reductions in resource and energy intensity to rapid economic growth driven by abundant fossil fuel exploitation. There is a greater than two‐fold difference in cumulative anthropogenic Hg emissions between the lower‐bound (110 Gg) and upper‐bound (235 Gg) scenarios. Hg releases to land and water are approximately six times those of direct emissions to air (600–1,470 Gg). At their peak, anthropogenic Hg emissions reach 2,200–2,600 Mg a−1 sometime between 2010 (baseline) and 2030, depending on the SSP scenario. Coal combustion is the largest determinant of differences in Hg emissions among scenarios. Decoupling of Hg and CO2 emission sources occurs under low‐to mid‐range scenarios, though contributions from artisanal and small‐scale gold mining remain uncertain. Future Hg emissions may have lower gaseous elemental Hg (Hg0) and higher divalent Hg (HgII), resulting in a higher fraction of locally sourced Hg deposition. Projected reemissions of previously deposited anthropogenic Hg follow a similar temporal trajectory to primary emissions, amplifying the benefits of primary Hg emission reductions under the most stringent mitigation scenarios.

Unveiling the Sources and Transfer of Mercury in Forest Bird Food Chains Using Techniques of Vivo-Nest Video Recording and Stable Isotopes.

Knowledge gaps in mercury (Hg) biomagnification in forest birds, especially in the most species-rich tropical and subtropical forests, limit our understanding of the ecological risks of Hg deposition to forest birds. This study aimed to quantify Hg bioaccumulation and transfer in the food chains of forest birds in a subtropical montane forest using a bird diet recorded by video and stable Hg isotope signals of biological and environmental samples. Results show that inorganic mercury (IHg) does not biomagnify along food chains, whereas methylmercury (MeHg) has trophic magnification factors of 7.4-8.1 for the basal resource-invertebrate-bird food chain. The video observations and MeHg mass balance model suggest that Niltava (Niltava sundara) nestlings ingest 78% of their MeHg from forest floor invertebrates, while Flycatcher (Eumyias thalassinus) nestlings ingest 59% from emergent aquatic invertebrates (which fly onto the canopy) and 40% from canopy invertebrates. The diet of Niltava nestlings contains 40% more MeHg than that of Flycatcher nestlings, resulting in a 60% higher MeHg concentration in their feather. Hg isotopic model shows that atmospheric Hg0 is the main Hg source in the forest bird food chains and contributes >68% in most organisms. However, three categories of canopy invertebrates receive ∼50% Hg from atmospheric Hg2+. Overall, we highlight the ecological risk of MeHg exposure for understory insectivorous birds caused by atmospheric Hg0 deposition and methylation on the forest floor.

Above- and belowground plant mercury dynamics in a salt marsh estuary in Massachusetts, USA

Abstract. Estuaries are a conduit of mercury (Hg) from watersheds to the coastal ocean, and salt marshes play an important role in coastal Hg cycling. Hg cycling in upland terrestrial ecosystems has been well studied, but processes in densely vegetated salt marsh ecosystems are poorly characterized. We investigated Hg dynamics in vegetation and soils in the Plum Island Sound estuary in Massachusetts, USA, and specifically assessed the role of marsh vegetation for Hg deposition and turnover. Monthly quantitative harvesting of aboveground biomass showed strong linear seasonal increases in Hg associated with plants, with a 4-fold increase in Hg concentration and an 8-fold increase in standing Hg mass from June (3.9 ± 0.2 µg kg−1 and 0.7 ± 0.4 µg m−2, respectively) to November (16.2 ± 2.0 µg kg−1 and 5.7 ± 2.1 µg m−2, respectively). Hg did not increase further in aboveground biomass after plant senescence, indicating physiological controls of vegetation Hg uptake in salt marsh plants. Hg concentrations in live roots and live rhizomes were 11 and 2 times higher than concentrations in live aboveground biomass, respectively. Furthermore, live belowground biomass Hg pools (Hg in roots and rhizomes, 108.1 ± 83.4 µg m−2) were more than 10 times larger than peak standing aboveground Hg pools (9.0 ± 3.3 µg m−2). A ternary mixing model of measured stable Hg isotopes suggests that Hg sources in marsh aboveground tissues originate from about equal contributions of root uptake (∼ 35 %), precipitation uptake (∼ 33 %), and atmospheric gaseous elemental mercury (GEM) uptake (∼ 32 %). These results suggest a more important role of Hg transport from belowground (i.e., roots) to aboveground tissues in salt marsh vegetation than upland vegetation, where GEM uptake is generally the dominant Hg source. Roots and soils showed similar isotopic signatures, suggesting that belowground tissue Hg mostly derived from soil uptake. Annual root turnover results in large internal Hg recycling between soils and plants, estimated at 58.6 µg m−2 yr−1. An initial mass balance of Hg indicates that the salt marsh presently serves as a small net Hg sink for environmental Hg of 5.2 µg m−2 yr−1.

Fate and Transport of Mercury through Waterflows in a Tropical Rainforest.

Knowledge gaps of mercury (Hg) biogeochemical processes in the tropical rainforest limit our understanding of the global Hg mass budget. In this study, we applied Hg stable isotope tracing techniques to quantitatively understand the Hg fate and transport during the waterflows in a tropical rainforest including open-field precipitation, throughfall, and runoff. Hg concentrations in throughfall are 1.5-2 times of the levels in open-field rainfall. However, Hg deposition contributed by throughfall and open-field rainfall is comparable due to the water interception by vegetative biomasses. Runoff from the forest shows nearly one order of magnitude lower Hg concentration than those in throughfall. In contrast to the positive Δ199Hg and Δ200Hg signatures in open-field rainfall, throughfall water exhibits nearly zero signals of Δ199Hg and Δ200Hg, while runoff shows negative Δ199Hg and Δ200Hg signals. Using a binary mixing model, Hg in throughfall and runoff is primarily derived from atmospheric Hg0 inputs, with average contributions of 65 ± 18 and 91 ± 6%, respectively. The combination of flux and isotopic modeling suggests that two-thirds of atmospheric Hg2+ input is intercepted by vegetative biomass, with the remaining atmospheric Hg2+ input captured by the forest floor. Overall, these findings shed light on simulation of Hg cycle in tropical forests.

Improving Simulation of Gas‐Particle Partitioning of Atmospheric Mercury Using CMAQ‐newHg‐Br v2

AbstractMercury (Hg) is a global pollutant whose atmospheric deposition is a major input to the terrestrial and oceanic ecosystems. Gas‐particle partitioning (GPP) of gaseous oxidized mercury (GOM) redistributes speciated Hg between gas and particulate phase and can subsequently alter Hg deposition flux. Most 3‐dimensional chemical transport models either neglected the Hg GPP process or parameterized it with measurement data limited in time and space. In this study, CMAQ‐newHg‐Br (Ye et al., 2018, https://doi.org/10.1002/2017ms001161) was updated to CMAQ‐newHg‐Br v2 by implementing a new GPP scheme and the most up‐to‐date Hg redox chemistry and was run for the northeastern United States over January‐November 2010. CMAQ‐newHg‐Br v2 reproduced the measured spatiotemporal distributions of gaseous elemental mercury (GEM) and particulate bound mercury (PBM) concentrations and Hg wet deposition flux within reasonable ranges and simulated dry deposition flux in agreement with previous studies. The GPP scheme improved the simulation of PBM via increasing winter‐, spring‐ and fall‐time PBM concentrations by threefold. It also improved simulated Hg wet deposition flux with an increase of 2.1 ± 0.7 μgm2 in the 11‐month accumulated amount, offsetting half of the decreasing effect of the updated chemistry (−4.2 ± 1.8 μgm2). Further, the GPP scheme captured the observed Kp‐T relationship as reported in previous studies without using measurement data and showed advantages at night and in rural/remote areas where existing empirical parameterizations failed. Our study demonstrated CMAQ‐newHg‐Br v2 a promising assessment tool to quantify impacts of climate change and emission reduction policy on Hg cycling.