Atmospheric Mercury Deposition Research Articles

Heavy metal pollution near an abandoned mercury-bearing waste recovery enterprise in southwestern China: Spatial distribution and its sources in soil and plants

The contribution of smelting of nonferrous metals to heavy metals in surface soil have become increasingly important over the past decade. In this study, the distribution of heavy metals around an abandoned mercury-bearing waste recovery enterprise were investigated. Soil (14) and plant (18) samples were collected in the surrounding area. The total concentration of heavy metals and methyl mercury content were measured by ICP-MS and HPLC-ICP-MS. The results show that the average contents of Cd, Cr, Pb, Hg and As in all soil samples are higher than the second-level values of Soil environmental quality-Risk control standard for soil contamination of development land (GB 36600-2018). Hg in the leaves ranged from 0.003 to 0.174 mg kg−1. Besides, the Pearson correlation analysis results indicate that Hg has a different environmental behavior compared to the other heavy metal under certain environmental or geographical conditions. But the mantel test statistical analysis results show that the Cr (P < 0.01), Cu, Pb, and Fe (P < 0.05) in the soil may have similar pollution sources with carbonate-bound mercury and iron-manganese oxide-bound mercury. The Hg concentrations show no correlation among plant leaves and soil, but significantly influenced by the distance and wind direction. These findings suggest that Hg in plant leaves may be derived from the deposition of atmospheric mercury from secondary mercury plant. The results will supplement those for relevant policy making for mercury-bearing waste recovery enterprises to improve urban environmental quality and human health.

Accumulation of total mercury in deep-sea sediments and biota across a bathymetric gradient in the Southeastern Mediterranean Sea

This study explores the accumulation of total mercury (THg) in deep-sea sediments and demersal megafauna of the ultra-oligotrophic Southeastern Mediterranean Sea (SEMS) across bathymetric gradients in the range 35–1900 m, sampled in seven cruises during 2013, 2017–2021, and 2023. Measurements of THg were conducted in surficial (0.0–0.5 cm) and subsurface (9.0–10 cm) sediments, demersal sharks, demersal teleost fish, and benthic crustaceans. Sedimentary organic carbon and biota δ13C and δ15N values were determined to explore possible foraging habitats and dietary sources of THg. The results exhibit an increasing trend of THg in surficial sediments with increasing bottom depth, while in the subsurface, pre-industrial sediments, THg remains lower, slightly increasing with depth. Having no major terrestrial point sources in this area, this increasing trend of THg in surficial sediments across bathymetric gradients is controlled by atmospheric mercury deposition, scavenged by the biological pump, and by lateral transport of particulate Hg in winnowed fine particles from the shelf. Similarly, the THg in benthic crustaceans and demersal fish ranged between 0.02 and 2.71 μg g−1 wet weight (0.06 and 10.8 μg g−1 dry weight) and increased with muscle δ13C as a function of distance offshore, while presenting a low THg-δ15N bio-magnification power. Our results suggest that foraging habitats, longevity, and species-specific depth distribution control their muscle THg bioaccumulation. Despite this complexity, the pooling of THg in megafauna into specific deep zones reflected the trend of increasing anthropogenic THg across bathymetric gradients. Furthermore, many of the biota measurements exceeded safe consumption thresholds for Hg and therefore, should be considered carefully in the development and regulation of deep-sea trawling in this region.

Mercury Isotope Composition in Open Water Corals of South China Sea: Implication for Atmospheric Mercury Deposition Pathways Into Tropical Oceans

AbstractThe deposition of different atmospheric mercury (Hg) species into oceans determines the atmospheric Hg lifetime and the production of neurotoxin methylmercury. Yet, the relative contribution of atmospheric Hg(II) and Hg(0) is largely unconstrained. Here, we report the concentrations of total Hg and methylmercury, as well as Hg isotope composition in living corals collected from the tropical South China Sea (SCS). The results show that the Hg in corals is mainly present as inorganic Hg, exhibiting slightly negative δ202Hg and small yet significant Δ199Hg and Δ200Hg. These isotope features closely resemble those of pelagic waters, suggesting that shallow‐water corals that are widely distributed in oligotrophic waters could be used to trace atmospheric Hg deposition pathways. A mixture model based on coral Δ200Hg indicates that approximately 49% of the seawater Hg in the tropical SCS, a region characterized by high rainfall, originates from atmospheric gaseous Hg(0), much larger than previous estimates.

Climatic regulation of atmospheric mercury deposition: Evidence from mercury isotopes in an alpine peat core

Abstract Mercury is a global pollutant that can undergo long-range transport in the atmosphere. While anthropogenic activities have largely increased atmospheric Hg emission and deposition since global industrialization, mechanisms governing the atmospheric Hg cycle in preindustrial periods remain unclear. Alpine peatlands receive Hg mainly from atmospheric Hg deposition and are sensitive to climatic changes, therefore alpine peat cores can be a useful archive for understanding the relationship between atmospheric Hg deposition and climate change. Here we reconstruct a 1200-year Hg deposition record based on a core drilled from an ombrotrophic peat bog in Yunnan-Guizhou Plateau, SW China. This core shows a dramatic change of Hg deposition fluxes (30.3–515 μg/m2/yr) associated with variable Hg isotopic composition (δ202Hg: –1.02‰ to –2.01‰; Δ199Hg: –0.16‰ to –0.50‰; Δ200Hg: –0.08‰ to 0.07‰). Using a Δ200Hg-based model, deposition fluxes of atmospheric Hg(0) and Hg(II) were estimated, which vary coherently with climatic indices (e.g., temperature, precipitation, and monsoon intensity). Results of this study imply that atmospheric Hg deposition in SW China is governed by two climate scenarios. In warm-house climates, low precipitation intensity and vegetation growth rates in SW China caused low atmospheric Hg(II) and Hg(0) deposition fluxes, respectively. In cold-house climates, high precipitation intensity and vegetation growth rates caused high atmospheric Hg(II) and Hg(0) deposition fluxes. This study highlights that climate changes can have a strong control on atmospheric Hg deposition.

Deposition and Re-Emission of Atmospheric Elemental Mercury over the Tropical Forest Floor.

Significant knowledge gaps exist regarding the emission of elemental mercury (Hg0) from the tropical forest floor, which limit our understanding of the Hg mass budget in forest ecosystems. In this study, biogeochemical processes of Hg0 deposition to and evasion from soil in a Chinese tropical rainforest were investigated using Hg stable isotopic techniques. Our results showed a mean air-soil flux as deposition of -4.5 ± 2.1 ng m-2 h-1 in the dry season and as emission of +7.4 ± 1.2 ng m-2 h-1 in the rainy season. Hg re-emission, i.e., soil legacy Hg evasion, induces negative transitions of Δ199Hg and δ202Hg in the evaded Hg0 vapor, while direct atmospheric Hg0 deposition does not exhibit isotopic fractionation. Using an isotopic mass balance model, direct atmospheric Hg0 deposition to soil was estimated to be 48.6 ± 13.0 μg m-2 year-1. Soil Hg0 re-emission was estimated to be 69.5 ± 10.6 μg m-2 year-1, of which 63.0 ± 9.3 μg m-2 year-1 is from surface soil evasion and 6.5 ± 5.0 μg m-2 year-1 from soil pore gas diffusion. Combined with litterfall Hg deposition (∼34 μg m-2 year-1), we estimated a ∼12.6 μg m-2 year-1 net Hg0 sink in the tropical forest. The fast nutrient cycles in the tropical rainforests lead to a strong Hg0 re-emission and therefore a relatively weaker atmospheric Hg0 sink.

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.

Quantifying Mercury Distribution and Source Contribution in Surface Soil of Qinghai-Tibetan Plateau Using Mercury Isotopes.

Long-range transport and atmospheric deposition of gaseous mercury (Hg0) result in significant accumulation of Hg in the Qinghai-Tibetan Plateau (QTP). However, there are significant knowledge gaps in understanding the spatial distribution and source contribution of Hg in the surface soil of the QTP and factors influencing Hg accumulation. In this study, we comprehensively investigated Hg concentrations and isotopic signatures in the QTP to address these knowledge gaps. Results show that the average Hg concentration in the surface soil ranks as follows: forest (53.9 ± 36.9 ng g-1) > meadow (30.7 ± 14.3 ng g-1) > steppe (24.5 ± 16.1 ng g-1) > shrub (21.0 ± 11.6 ng g-1). Hg isotopic mass mixing and structural equation models demonstrate that vegetation-mediated atmospheric Hg0 deposition dominates the Hg source in the surface soil, with an average contribution of 62 ± 12% in forests, followed by 51 ± 10% in shrub, 50 ± 13% in steppe, and 45 ± 11% in meadow. Additionally, geogenic sources contribute 28-37% of surface soil Hg accumulation, and atmospheric Hg2+ inputs contribute 10-18% among the four types of biomes. The Hg pool in 0-10 cm surface soil over the QTP is estimated as 8200 ± 3292 Mg. Global warming, permafrost degradation, and anthropogenic influences have likely perturbed Hg accumulation in the soil of QTP.

Dry and Wet Deposition Fluxes and Source of Atmospheric Mercury in the Forest in Southeast China

Studying atmospheric mercury (Hg) deposition in a forest system is a key step to understanding Hg biogeochemical cycles. However, observations based on Hg deposition fluxes in worldwide stations under forest ecosystems tend to differ considerably. In this work, a sampling station was set up in Dinghu Mountain to study the atmospheric Hg’s dry and wet deposition in typical forest ecosystems in Southeast China. One hundred and two atmospheric dry and wet deposition samples were collected with an automatic sampler from March 2009 to February 2010, and concentrations of Hg, magnesium (Mg), calcium (Ca), cadmium (Cd), copper (Cu), zinc (Zn), lead (Pb), and chromium (Cr) were detected. The results showed that the annual rainfall weighted average Hg concentration was 56.8 ng L−1, and 79.8 ng L−1 in the dry deposition. The mean total deposition flux was 158.8 μg m−2, and the wet deposition was predominant. The highest and lowest concentrations were detected in the high-temperature rainy season. Generally, the wet deposition flux was notably positively correlated with the rainfall. The source of atmospheric Hg deposition in Dinghu Mountain was analyzed using principal component analysis (PCA). The main source of Hg in precipitation was soil dust, followed by coal and fuel (automobile exhaust). The primary source of Hg in dry deposition was fuel (automobile exhaust), followed by soil dust, which indicates that Dinghu Mountain has been polluted by the anthropogenic sources of Hg.

Atmospheric wet deposition of mercury in urban Jinan, eastern China: Speciation, scavenging process and potential sources

Understanding the speciation and related influence factors of Hg in wet deposition is important to predict the fate and transport of mercury in the atmosphere. In this study, event-based samples of rainwater were collected for one year in Jinan, a northern city in eastern China. The volume-weighted mean concentration of total mercury (THg) in rainwater was 34.8 ng L−1, comparable to levels in some inland cities in China and were significantly higher than those in North America, Korea and Japan. Most of the Hg in rainwater was associated with particulates, accounted for 15.2–92.9% of THg with a mean of 66.9%, which might be attributed to the scavenging effects of high particulate-bound mercury concentrations in ambient air in urban Jinan. Dissolved mercury (DHg) accounted for 33.1% of THg, in which Hg(OH)2, HgClOH, HgCl2 and Hg(NH3)22+ are the dominant species based on the chemical equilibrium modeling simulations. THg concentrations in rainwater decreased as the rainfall amount increased owing to the dilution effect and 5 mm rainfall might be a threshold for the full wash-out capability of atmospheric Hg. For a continuous rain event, the proportion of DHg in THg could increase from 7.1% to 84.8% with the rainfall processing, especially for the species of HgClOH and HgCl2 under the influence of rainwater pH. Positive matrix factorization (PMF) analysis suggested that the major sources of Hg in rainwater were combustion emissions, marine sources, industrial emissions, as well as complexation process, which contributed to 51.4%, 24.7%, 12.2%, and 11.7% of the THg, respectively. For the specific species, the main sources varied with different Hg species, in which combustion emissions contributed one third to one half of each species sum to particulate mercury (PHg), HgClOH, HgCl2, HgBrOH and HgBrCl followed by marine sources and industrial emissions. Cluster analysis of backward trajectories revealed that polluted air masses, transported from southeast Shandong, Anhui and Jiangsu Provinces, as well as Beijing-Tianjin-Hebei region, contributed to high Hg concentration in rainwater in Jinan.

Mosses and lichens enhance atmospheric elemental mercury deposition in a subtropical montane forest†

Environmental context Mosses and lichens are widely distributed in montane forests and their important role in global biogeochemical cycles has been increasingly recognised. This study of mercury accumulation and sources in mosses and lichens, using mercury isotopic data, provides evidence that they promote atmospheric mercury deposition in these forests, which is an important function that should be incorporated into current mercury mass balance budgets for forests. Rationale Mosses and lichens, which are widely distributed in montane forests, are often used to monitor the atmospheric mercury (Hg) depositions. In this study we hypothesised that atmospheric Hg uptake by mosses and lichens could greatly promote Hg depositions in montane forests. Methodology We comprehensively determined the Hg concentration and isotopic signatures of various species of mosses and lichens in a subtropical montane forest, to quantify the Hg accumulation, influencing factors and potential Hg depositions induced by mosses and lichens. Results Our results show that the higher Hg concentrations in mosses than in lichens are mainly due to their species-specific, morphological and physiological differences. Hg isotopic mixing model results display that uptake of atmospheric elemental Hg (Hg0) contributes 89.2 ± 22.8% of Hg in mosses and 88.4 ± 24.4% in lichens. The lichens growing on trees have a lower atmospheric Hg0 source contribution than on the ground (61.3 ± 42.5% versus 93.6 ± 10.0%) because of the elevated rainfall Hg uptake on trees. The Hg storage in live moss and lichen is 28.0 ± 16.5 and 0.9 ± 1.0 μg m−2, respectively. Given the 1–2-year lifespan of moss, the moss induced atmospheric Hg deposition is almost equivalent to litterfall Hg deposition which was previously used as a proxy for atmospheric Hg0 deposition in forests. Discussion Overall, we suggest mosses and lichens play an important role in atmospheric Hg depositions and recommend more research in montane forests.

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.

Mercury in soil, sediment, and lake water in upland headwater catchments in Ireland

Mercury concentrations in the atmosphere, surface waters, and soils have increased beyond natural levels as a result of human activities, which poses a risk to human and environmental health. Ireland is situated on the western periphery of Europe, and it is generally assumed that environmental mercury is low but there is limited information on mercury within natural environments. In this study, the interlinkages in the concentration of mercury in soils, lake sediment, and lake water were investigated in remote upland acid-sensitive catchments influenced by low deposition of atmospheric mercury. Thirty-one upland lake catchments were sampled for topsoil, lake sediment, and lake water during 2017–2018. Total mercury (THg) concentrations in water (median 5.4 ng/L) and sediment (median 30 ng/g) were low, owing to the remote location of the lakes. In contrast, THg in catchment soil was relatively high for a background region (median: 240 ng/g), which was attributed to the high organic matter content of the soil (median 87%). The results suggest catchment soils are the dominant driver of variation in THg in lake water and sediment in upland regions in Ireland. Further, given that highly organic soils can obscure interlinkages within catchments, this study demonstrated the value of exploring mercury independent of the influence of organic matter, i.e., THg normalized by organic carbon. As global action (such as the Minamata Convention) decreases mercury emissions, legacy soil mercury may become a more important input to aquatic systems than atmospheric deposition, which makes the relationships between terrestrial catchments and their water bodies vital for our understanding of mercury cycling.

Updated trends for atmospheric mercury in the Arctic: 1995-2018.

The Arctic region forms a unique environment with specific physical, chemical, and biological processes affecting mercury (Hg) cycles and limited anthropogenic Hg sources. However, historic global emissions and long range atmospheric transport has led to elevated Hg in Arctic wildlife and waterways. Continuous atmospheric Hg measurements, spanning 20 years, and increased monitoring sites has allowed a more comprehensive understanding of how Arctic atmospheric mercury is changing over time. Time-series trend analysis of TGM (Total Gaseous Mercury) in air was performed from 10 circumpolar air monitoring stations, comprising of high-Arctic, and sub-Arctic sites. GOM (gaseous oxidised mercury) and PHg (particulate bound mercury) measurements were also available at 2 high-Arctic sites. Seasonal mean TGM for sub-Arctic sites were lowest during fall ranging from 1.1 ng m-3 Hyytiälä to 1.3 ng m-3, Little Fox Lake. Mean TGM concentrations at high-Arctic sites showed the greatest variability, with highest daily means in spring ranging between 4.2 ng m-3 at Amderma and 2.4 ng m-3 at Zeppelin, largely driven by local chemistry. Annual TGM trend analysis was negative for 8 of the 10 sites. High-Arctic seasonal TGM trends saw smallest decline during summer. Fall trends ranged from -0.8% to -2.6% yr-1. Across the sub-Arctic sites spring showed the largest significant decreases, ranging between -7.7% to -0.36% yr-1, while fall generally had no significant trends. High-Arctic speciation of GOM and PHg at Alert and Zeppelin showed that the timing and composition of atmospheric mercury deposition events are shifting. Alert GOM trends are increasing throughout the year, while PHg trends decreased or not significant. Zeppelin saw the opposite, moving towards increasing PHg and decreasing GOM. Atmospheric mercury trends over the last 20 years indicate that Hg concentrations are decreasing across the Arctic, though not uniformly. This is potentially driven by environmental change, such as plant productivity and sea ice dynamics.

Effect of Land Cover on Ecoregion-Scale Spatial Patterns of Mercury Contamination of Largemouth Bass in the Southeastern United States.

Consumption of methylmercury (MeHg)-contaminated fish is the primary source of MeHg in humans and poses a hazard to human health. Because of widespread atmospheric deposition of inorganic mercury (IHg), all water bodies in the United States have been contaminated with Hg. In aquatic ecosystems, IHg is converted to MeHg, which biomagnifies, reaching high concentrations in piscivorous fish. It is not possible for governmental agencies to monitor fish from every waterbody to determine if concentrations of MeHg in fish are hazardous to human health. To help government agencies focus their monitoring efforts, it is critical that we develop the ability to predict regions where waterbodies are most likely to contain fish with hazardous concentrations of MeHg. The objective of the present study was to examine the relationship between MeHg contamination of largemouth bass (Micropterus salmoides), a popular piscivorous gamefish, and land cover in 24 ecoregions across 15 states in the southeastern United States. In our study we demonstrate for the first time that 72% of the variance in average concentrations of MeHg in largemouth bass between ecoregions of the southeastern United States can be explained by the percentage coverage by evergreen forests, emergent herbaceous wetlands, and pasture/hay. Land cover determines the sensitivity of freshwater systems to atmospheric IHg deposition, and the present study suggests that at the ecoregion scale, MeHg bioaccumulation in piscivorous gamefish, and ultimately the health hazard that these MeHg-contaminated fish pose to humans, can be in part predicted by land-cover type. Environ Toxicol Chem 2022;41:2386-2394. © 2022 SETAC.

The interplay between atmospheric deposition and soil dynamics of mercury in Swiss and Chinese boreal forests: A comparison study

Taking advantage of the different histories of Hg deposition in Davos Seehornwald in E-Switzerland and Changbai Mountain in NE-China, the influence of atmospheric deposition on Hg soil dynamics in forest soil profiles was investigated. Today, Hg fluxes in bulk precipitation were similar, and soil profiles were generally sinks for atmospherically deposited Hg at both sites. Noticeably, a net release of 2.07 μg Hg m−2 yr−1 from the Bs horizon (Podzol) in Seehornwald was highlighted, where Hg concentration (up to 73.9 μg kg−1) and soil storage (100 mg m−3) peaked. Sequential extraction revealed that organic matter and crystalline Fe and Al hydr (oxide)-associated Hg decreased in the E horizon but increased in the Bs horizon as compared to the Ah horizon, demonstrating the coupling of Hg dynamics with the podzolisation process and accumulation of legacy Hg deposited last century in the Bs horizon. The mor humus in Seehornwald allowed Hg enrichment in the forest floor (182–269 μg kg−1). In Changbai Mountain, the Hg concentrations in the Cambisol surface layer with mull humus were markedly lower (<148 μg kg−1), but with much higher Hg soil storage (54–120 mg m−3) than in the Seehornwald forest floor (18–27 mg m−3). Thus, the vertical distribution pattern of Hg was influenced by humus form and soil type. The concentrations of Hg in soil porewater in Seehornwald (3.4–101 ng L−1) and in runoff of Changbai Mountain (1.26–5.62 ng L−1) were all low. Moreover, the pools of readily extractable Hg in the soils at both sites were all <2% of total Hg. Therefore, the potential of Hg release from the forest soil profile to the adjacent aquatic environment is currently low at both sites.

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.

Improved atmospheric mercury simulation using updated gas-particle partition and organic aerosol concentrations

The gaseous or particulate forms of divalent mercury (HgII) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux (FLX). In the new nested-grid GEOS-Chem model, we try to modify the HgII gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg (GOM), particulate-bound Hg (PBM), and PM2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature (T) and organic aerosol (OA) concentrations under different relative humidity (RH). Results showed that with increasing RH, the dominant process of HgII gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of HgII gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases (NMBs) of monthly gaseous element mercury (GEM), GOM, PBM, WFLX were reduced from −33%–29%, 95%–300%, 64%–261%, 117%–122% to −13%–0%, −20%–80%, −31%–50%, −17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.

Caribbean Lead and Mercury Pollution Archived in a Crater Lake.

Lead and mercury have long histories of anthropogenic use and release to the environment extending into preindustrial times. Yet, the timing, magnitude, and persistence of preindustrial emissions remain enigmatic, especially for mercury. Here, we quantify tropical lead and mercury deposition over the past ∼3000 years using a well-dated sediment core from a small crater lake (Lake Antoine, Grenada). Preindustrial increases in lead and mercury concentrations can be explained by varying inputs of watershed mineral and organic matter, which in turn reflect climate-driven changes in the lake level. We find no evidence that preindustrial lead and mercury use raised deposition rates in this remote ecosystem, and our results underscore the need to carefully evaluate common normalization approaches for changing lithogenic inputs and sedimentation rates. Industrial-era lead and mercury accumulation rates in Lake Antoine have been accelerated by land use and land cover change within the crater rim, yet global industrial pollution remains evident. After correcting for watershed inputs, we find that recent atmospheric lead and mercury deposition rates averaged 2925 and 24 μg/m2/y, respectively, which are in close agreement with monitoring data. Our results challenge recent assessments suggesting preindustrial mercury use raised atmospheric deposition rates globally, highlighting the unique nature of 20th Century industrial pollution.

Tracing the Transboundary Transport of Mercury to the Tibetan Plateau Using Atmospheric Mercury Isotopes

Deposition of atmospheric mercury (Hg) is the most important Hg source on the high-altitude Himalayas and Tibetan Plateau. Herein, total gaseous Hg (TGM) at an urban and a forest site on the Tibetan Plateau was collected respectively from May 2017 to October 2018, and isotopic compositions were measured to clarify the influences of landforms and monsoons on the transboundary transport of atmospheric Hg to the Tibetan Plateau. The transboundary transported anthropogenic emissions mainly originated over Indo-Gangetic Plain and carried over the Himalayas by convective storms and mid-tropospheric circulation, contributing over 50% to the TGM at the Lhasa urban site, based on the binary mixing model of isotopes. In contrast, during the transport of TGM from South Asia with low altitude, the uptake by evergreen forest in Yarlung Zangbo Grand Canyon largely decreased the TGM level and shifted isotopic compositions in TGM at the Nyingchi forest site, which are located at the high-altitude end of the canyon. Our results provided direct evidence from Hg isotopes to reveal the distinct patterns of transboundary transport to the Tibetan Plateau shaped by landforms and climates, which is critical to fully understand the biogeochemical cycling of Hg in the high-altitude regions.

The Interplay between Atmospheric Deposition and Soil Dynamics of Mercury in Swiss and Chinese Boreal Forests: A Comparison Study

The Interplay between Atmospheric Deposition and Soil Dynamics of Mercury in Swiss and Chinese Boreal Forests: A Comparison Study