Isotope Data Constrains Redox Chemistry of Atmospheric Mercury.

The redox chemistry of mercury (Hg) in the atmosphere exerts a significant influence on its global cycle. However, our understanding of this important process remains shrouded in uncertainty. In this study, we utilize three-dimensional atmospheric Hg isotope modeling to evaluate the isotopic composition of particle-bound mercury [HgII(P)] in the global atmosphere. We investigate various chemistry mechanisms and find that they induce remarkably disparate odd-number mass-independent fractionation (odd-MIF) in HgII(P) on a global scale. The observed odd-MIF data identify the essential role of sea salt aerosol debromination in the redox chemistry of atmospheric Hg and underscore the predominant influence of Br oxidation in the marine boundary layer. The odd-MIF signatures significantly narrow the uncertainty range of redox chemistry rates and constrain the photoreduction of HgII(P) at a magnitude of 10-3 JNO2 (local photolysis frequency of NO2) in the global atmosphere. This study advances our understanding of atmospheric Hg chemistry processes and provides insights into the potential impacts of climate change on Hg cycling.

Potential decoupling of CO2 and Hg uptake process by global vegetation in the 21st century.

Mercury (Hg), a potent neurotoxin posing risks to human health, is cycled through vegetation uptake, which is susceptible to climate change impacts. However, the extent and pattern of these impacts are largely unknown, obstructing predictions of Hg's fate in terrestrial ecosystems. Here, we evaluate the effects of climate change on vegetation elemental Hg [Hg(0)] uptake using a state-of-the-art global terrestrial Hg model (CLM5-Hg) that incorporates plant physiology. In a business-as-usual scenario, the terrestrial Hg(0) sink is predicted to decrease by 1870 Mg yr-1 in 2100, that is ~60% lower than the present-day condition. We find a potential decoupling between the trends of CO2 assimilation and Hg(0) uptake process by vegetation in the 21st century, caused by the decreased stomatal conductance with increasing CO2. This implies a substantial influx of Hg into aquatic ecosystems, posing an elevated threat that warrants consideration during the evaluation of the effectiveness of the Minamata Convention.

Modeling the Mercury Cycle in the Sea Ice Environment: A Buffer between the Polar Atmosphere and Ocean.

Sea ice (including overlying snow) is a dynamic interface between the atmosphere and the ocean, influencing the mercury (Hg) cycling in polar oceans. However, a large-scale and process-based model for the Hg cycle in the sea ice environment is lacking, hampering our understanding of regional Hg budget and critical processes. Here, we develop a comprehensive model for the Hg cycle at the ocean-sea ice-atmosphere interface with constraints from observational polar cryospheric data. We find that seasonal patterns of average total Hg (THg) in snow are governed by snow thermodynamics and deposition, peaking in springtime (Arctic: 5.9 ng/L; Antarctic: 5.3 ng/L) and minimizing during ice formation (Arctic: 1.0 ng/L, Antarctic: 0.5 ng/L). Arctic and Antarctic sea ice exhibited THg concentration peaks in summer (0.25 ng/L) and spring (0.28 ng/L), respectively, governed by different snow Hg transmission pathways. Antarctic snow-ice formation facilitates Hg transfer to sea ice during spring, while in the Arctic, snow Hg is primarily moved through snowmelt. Overall, first-year sea ice acts as a buffer, receiving atmospheric Hg during ice growth and releasing it to the ocean in summer, influencing polar atmospheric and seawater Hg concentrations. Our model can assess climate change effects on polar Hg cycles and evaluate the Minamata Convention's effectiveness for Arctic populations.

Mercury budgets in the suspended particulate matters of the Yangtze River.

Riverine processes are crucial for the biogeochemical cycle of mercury (Hg). The Yangtze River, the largest river in East Asia, discharges a substantial amount of Hg into the East China Sea. However, the influencing factors of the Hg budget and its recent trends remain unclear. This study quantitatively analyzed the total Hg concentration (THg) in suspended particulate matter (SPM) in the Yangtze River and calculated the Hg budget in 2018 and 2021. The results showed that the total Hg concentrations varied substantially along the river, with concentrations ranging from 23 to 883 µg/kg in 2018 and 47 to 146 µg/kg in 2021. The average Hg flux to China Sea in 2018 and 2021 were approximately 10 Mg/yr, lower than in 2016 (48 Mg/yr). Over 70% of the SPM was trapped in the Three Gorges Dam (TGD), and 22 Mg/yr of Hg settled in the TGD in 2018 and 10 Mg/yr in 2021. Hg fluxes in the Yangtze River watershed were driven by various factors, including decreased industrial emissions, increased agriculture emissions, and decreased soil erosion flux. We found that in the upper reach of the Yangtze River changed from sink to source of Hg possibly due to the resuspension of sediments, which implies that the settled sediments could be a potential source of Hg for downstream. Overall, emission control policies may have had a positive impact on reducing Hg flux to the East China Sea from 2016 to 2021, but more efforts are needed to further reduce Hg emissions.

International trade shapes global mercury-related health impacts.

Mercury (Hg) is a strong neurotoxin with substantial dangers to human health. Hg undergoes active global cycles, and the emission sources there of can also be geographically relocated through economic trade. Through investigation of a longer chain of the global biogeochemical Hg cycle from economic production to human health, international cooperation on Hg control strategies in Minamata Convention can be facilitated. In the present study, four global models are combined to investigate the effect of international trade on the relocation of Hg emissions, pollution, exposure, and related human health impacts across the world. The results show that 47% of global Hg emissions are related to commodities consumed outside of the countries where the emissions are produced, which has largely influenced the environmental Hg levels and human exposure thereto across the world. Consequently, international trade is found to enable the whole world to avoid 5.7 × 105 points for intelligence quotient (IQ) decline and 1,197 deaths from fatal heart attacks, saving a total of $12.5 billion (2020 USD) in economic loss. Regionally, international trade exacerbates Hg challenges in less developed countries, while resulting in an alleviation in developed countries. The change in economic loss therefore varies from the United States (-$4.0 billion) and Japan (-$2.4 billion) to China (+$2.7 billion). The present results reveal that international trade is a critical factor but might be largely overlooked in global Hg pollution mitigation.

Buffering effect of global vegetation on the air-land exchange of mercury: Insights from a novel terrestrial mercury model based on CESM2-CLM5.

The vegetation uptake of atmospheric elemental mercury [Hg(0)] and its subsequent littering are critical processes of the terrestrial Hg cycles. There is a large uncertainty in the estimated global fluxes of these processes due to the knowledge gap in the underlying mechanisms and their relationship with environmental factors. Here, we develop a new global model based on the Community Land Model Version 5 (CLM5-Hg) as an independent component of the Community Earth System Model 2 (CESM2). We explore the global pattern of gaseous elemental Hg [Hg(0)] uptake by vegetation and the spatial distribution of litter Hg concentration constrained by observed datasets as well as its driving mechanism. The annual vegetation uptake of Hg(0) is estimated as 3132 Mg yr-1, which is considerably higher than previous global models. The scheme of dynamic plant growth including stomatal activities substantially improves the estimation for global terrestrial distribution of Hg, compared to the leaf area index (LAI) based scheme that is often used by previous models. We find the global distribution of litter Hg concentrations driven by vegetation uptake of atmospheric Hg(0), which are simulated to be higher in East Asia (87 ng/g) than in the Amazon region (63 ng/g). Meanwhile, as a significant source for litter Hg, the formation of structural litter (cellulose litter + lignin litter) results in a lagging effect between Hg(0) deposition and litter Hg concentration, implying the buffering effect of vegetation on the air-land exchange of Hg. This work highlights the importance of vegetation physiology and environmental factors in understanding the vegetation sequestration of atmospheric Hg globally, and calls for greater efforts to protect forests and afforestation.

Modeling mercury isotopic fractionation in the atmosphere.

Mercury (Hg) stable isotope analysis has become a powerful tool to identify Hg sources and to understand its biogeochemical processes. However, it is challenging to link the observed Hg isotope fractionation to its global cycling. Here, we integrate source Hg isotope signatures and process-based Hg isotope fractionation into a three-dimensional isotope model based on the GEOS-Chem model platform. Our simulated isotope compositions of total gaseous Hg (TGM) are broadly comparable with available observations across global regions. The isotope compositions of global TGM, potentially distinguishable over different regions, are caused by the atmospheric mixture of anthropogenic, natural, and re-emitted Hg sources, superimposed with competing processes, notably gaseous Hg(0) dry deposition and Hg redox transformations. We find that Hg(0) dry deposition has a great impact on the isotope compositions of global TGM and drives the seasonal variation of δ202Hg in forest-covered regions. The atmospheric photo-reduction of Hg(Ⅱ) dominates over Hg(0) oxidation in driving the global Δ199Hg (and Δ201Hg) distribution patterns in TGM. We suggest that the magnitude of isotope fractionation associated with atmospheric aqueous-phase Hg(Ⅱ) reduction is likely close to aquatic Hg(Ⅱ) reduction. Our model provides a vital tool for coupling the global atmospheric Hg cycle and its isotope fractionation at various scales and advances our understanding of atmospheric Hg transfer and transformation mechanisms.

Heavy Metal in Rice and Vegetable and Human Exposure near a Large Pb/Zn Smelter in Central China.

Non-ferrous metal smelting is a significant source of anthropogenic heavy metal emission and has led to severe environmental pollution that ultimately threatens the health of local residents. In this study, we determined concentrations of copper (Cu), zinc (Zn), cadmium (Cd) and lead (Pb), as well as Pb isotopic compositions in rice, vegetables and human hair in areas surrounding the Zhuzhou Pb/Zn smelter in Hunan, China and we assessed the health risks associated with rice and vegetable consumption for local residents. Results showed that rice and vegetable samples were significantly contaminated by Cd and Pb. Age and source of rice were important factors for the enrichment of heavy metal concentrations in human hair. The ratios of Pb isotopes in human hair (1.164-1.170 for 206Pb/207Pb and 2.102-2.110 for208Pb/206Pb) were comparable to those in rice (1.162-1.172 for 206Pb/207Pb and 2.098-2.114 for208Pb/206Pb) and were slightly lower than those in vegetables (1.168-1.172 for 206Pb/207Pb and 2.109-2.111 for208Pb/206Pb), indicating that Pb in human hair mainly originated from food ingestion. A non-carcinogenic risk assessment showed that Cd exposure was the dominant health risk for local residents. This study suggested that crops planted surrounding the smelter were seriously contaminated with Cd and human exposure was related to dietary intake.

Global health effects of future atmospheric mercury emissions.

Mercury is a potent neurotoxin that poses health risks to the global population. Anthropogenic mercury emissions to the atmosphere are projected to decrease in the future due to enhanced policy efforts such as the Minamata Convention, a legally-binding international treaty entered into force in 2017. Here, we report the development of a comprehensive climate-atmosphere-land-ocean-ecosystem and exposure-risk model framework for mercury and its application to project the health effects of future atmospheric emissions. Our results show that the accumulated health effects associated with mercury exposure during 2010-2050 are $19 (95% confidence interval: 4.7-54) trillion (2020 USD) realized to 2050 (3% discount rate) for the current policy scenario. Our results suggest a substantial increase in global human health cost if emission reduction actions are delayed. This comprehensive modeling approach provides a much-needed tool to help parties to evaluate the effectiveness of Hg emission controls as required by the Minamata Convention.

Mercury speciation and mobility in salt slurry and soils from an abandoned chlor-alkali plant, Southwest China.

Chlor-alkali plants (CAPs) are major consumers of mercury (Hg) and may be a source of severe Hg pollution to the environment. In this paper, the total mercury (THg) concentrations and the speciation and mobility of Hg were measured in salt slurry and soils collected from an abandoned CAP in Yunnan Province, China. THg concentrations in the salt slurry samples varied widely and ranged from 0.43 to 2640 mg/kg; THg concentrations varied vertically and were lower towards the surface than deeper in the profile. In the soils, a sample collected from electrolysis workshop had the highest THg concentration (3650 mg/kg). The main fractions of Hg in the salt slurry and soils were Hg2+ and Hg0, which accounted for 47.4% and 22.9% of THg in the salt slurry and 28.0% and 43.8% of THg in the soils on average, respectively. The Hg0 concentrations decreased with depth in the soil profiles. The total soluble Hg (TSHg) concentrations in the salt slurry averaged at 140 µg/L and ranged from 0.77 to 564 µg/L. The salt slurry and soils at the study site were seriously contaminated with Hg, which could potentially be released to the atmosphere or water bodies.

Effect of Al Element on the Microstructure and Properties of Cu-Ni-Fe-Mn Alloys.

The effects of aluminum on the mechanical properties and corrosion behavior in artificial seawater of Cu-Ni-Fe-Mn alloys were investigated. Cu-7Ni-xAl-1Fe-1Mn samples, consisting of 0, 1, 3, 5, and 7 wt % aluminum along with the same contents of other alloying elements (Ni, Fe, and Mn), were prepared. The microstructure of Cu-7Ni-xAl-1Fe-1Mn alloy was analyzed by Transmission Electron Microscopy (TEM), and its corrosion property was tested by an electrochemical system. The results show that the mechanical and corrosion properties of Cu-7Ni-xAl-1Fe-1Mn alloy have an obvious change with the aluminum content. The tensile strength has a peak value of 395 MPa by adding 3 wt % aluminum in the alloy. Moreover, the corrosion rate in artificial seawater of Cu-7Ni-3Al-1Fe-1Mn alloy is 0.0215 mm/a which exhibits a better corrosion resistance than the commercially used UNS C70600. It is confirmed that the second-phase transformation of Cu-7Ni-xAl-1Fe-1Mn alloy follows the sequence of α solid solution → Ni3Al → Ni3Al + NiAl → Ni3Al + NiAl3. The electrochemical impedance spectroscopy (EIS) shows that the adding element aluminum in the Cupronickel can improve the corrosion resistance of Cu-7Ni-xAl-1Fe-1Mn alloy.