Photoreduction of gaseous oxidized mercury changes global atmospheric mercury speciation, transport and deposition.
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ABSTRACT:
SUBMITTER: Saiz-Lopez A
PROVIDER: S-EPMC6237998 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Understanding atmospheric mercury chemistry is the key for explaining the biogeochemical cycle of mercury and for improving the predictive capability of computational models. Increased efforts are being made to ensure comparable Hg speciation measurements in the air through establishing metrological traceability. While traceability for elemental mercury has been recently set, this is by no means the case for gaseous oxidized mercury (GOM). Since a calibration unit suitable for traceable GOM calibrations based on evaporation of HgCl2 solution was recently developed, the purpose of our work was to extensively evaluate its performance. A highly specific and sensitive 197Hg radiotracer was used for validation over a wide range of concentrations. By comparing experimental and calculated values, we obtained recoveries for the calibration unit. The average recoveries ranged from 88.5% for 1178 ng m-3 HgCl2 gas concentration to 39.4% for 5.90 ng m-3 HgCl2 gas concentration. The losses were due to the adsorption of oxidized Hg on the inner walls of the calibrator and tubing. An adsorption isotherm was applied to estimate adsorption enthalpy (ΔHads); a ΔHads value of -12.33 kJ mol-1 was obtained, suggesting exothermal adsorption. The results of the calibrator performance evaluation suggest that a newly developed calibration unit is only suitable for concentrations of HgCl2 higher than 1 µg m-3. The concentration dependence of recoveries prevents the system from being used for calibration of instruments for ambient GOM measurements. Moreover, the previously assessed uncertainty of this unit at µg m-3 level (2.0%, k = 2) was re-evaluated by including uncertainty related to recovery and was found to be 4.1%, k = 2. Calibrator performance was also evaluated for HgBr2 gas calibration; the recoveries were much lower for HgBr2 gas than for HgCl2 gas even at a high HgBr2 gas concentration (>1 µg m-3). As HgBr2 is often used as a proxy for various atmospheric HgBr species, the suitability of the unit for such calibration must be further developed.
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Project description:Atmospheric mercury measurements carried out in the recent decades have been a subject of bias largely due to insufficient consideration of metrological traceability and associated measurement uncertainty, which are ultimately needed for the demonstration of comparability of the measurement results. This is particularly challenging for gaseous HgII species, which are reactive and their ambient concentrations are very low, causing difficulties in proper sampling and calibration. Calibration for atmospheric HgII exists, but barriers to reliable calibration are most evident at ambient HgII concentration levels. We present a calibration of HgII species based on nonthermal plasma oxidation of Hg0 to HgII. Hg0 was produced by quantitative reduction of HgII in aqueous solution by SnCl2 and aeration. The generated Hg0 in a stream of He and traces of reaction gas (O2, Cl2, or Br2) was then oxidized to different HgII species by nonthermal plasma. A highly sensitive 197Hg radiotracer was used to evaluate the oxidation efficiency. Nonthermal plasma oxidation efficiencies with corresponding expanded standard uncertainty values were 100.5 ± 4.7% (k = 2) for 100 pg of HgO, 96.8 ± 7.3% (k = 2) for 250 pg of HgCl2, and 77.3 ± 9.4% (k = 2) for 250 pg of HgBr2. The presence of HgO, HgCl2, and HgBr2 was confirmed by temperature-programmed desorption quadrupole mass spectrometry (TPD-QMS). This work demonstrates the potential for nonthermal plasma oxidation to generate reliable and repeatable amounts of HgII compounds for routine calibration of ambient air measurement instrumentation.
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Project description:Gaseous oxidized mercury (GOM) dry deposition measurements using aerodynamic surrogate surface passive samplers were collected in central and eastern Texas and eastern Oklahoma, from September 2011 to September 2012. The purpose of this study was to provide an initial characterization of the magnitude and spatial extent of ambient GOM dry deposition in central and eastern Texas for a 12-month period which contained statistically average annual results for precipitation totals, temperature, and wind speed. The research objective was to investigate GOM dry deposition in areas of Texas impacted by emissions from coal-fired utility boilers and compare it with GOM dry deposition measurements previously observed in eastern Oklahoma and the Four Corners area. Annual GOM dry deposition rate estimates were relatively low in Texas, ranging from 0.1 to 0.3 ng/m(2)h at the four Texas monitoring sites, similar to the 0.2 ng/m(2)h annual GOM dry deposition rate estimate recorded at the eastern Oklahoma monitoring site. The Texas and eastern Oklahoma annual GOM dry deposition rate estimates were at least four times lower than the highest annual GOM dry deposition rate estimate previously measured in the more arid bordering western states of New Mexico and Colorado in the Four Corners area.
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Project description:Mercury is toxic to wildlife and humans, and forests are thought to be a globally important sink for gaseous elemental mercury (GEM) deposition from the atmosphere. Yet there are currently no annual GEM deposition measurements over rural forests. Here we present measurements of ecosystem-atmosphere GEM exchange using tower-based micrometeorological methods in a midlatitude hardwood forest. We measured an annual GEM deposition of 25.1 µg ⋅ m-2 (95% CI: 23.2 to 26.7 1 µg ⋅ m-2), which is five times larger than wet deposition of mercury from the atmosphere. Our observed annual GEM deposition accounts for 76% of total atmospheric mercury deposition and also is three times greater than litterfall mercury deposition, which has previously been used as a proxy measure for GEM deposition in forests. Plant GEM uptake is the dominant driver for ecosystem GEM deposition based on seasonal and diel dynamics that show the forest GEM sink to be largest during active vegetation growing periods and middays, analogous to photosynthetic carbon dioxide assimilation. Soils and litter on the forest floor are additional GEM sinks throughout the year. Our study suggests that mercury loading to this forest was underestimated by a factor of about two and that global forests may constitute a much larger global GEM sink than currently proposed. The larger than anticipated forest GEM sink may explain the high mercury loads observed in soils across rural forests, which impair water quality and aquatic biota via watershed Hg export.
| S-EPMC8307844 | biostudies-literature
Project description: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.
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Project description:The Adirondacks of New York State, USA is a region that is sensitive to atmospheric mercury (Hg) deposition. In this study, we estimated atmospheric Hg deposition to the Adirondacks using a new scheme that combined numerical modeling and limited experimental data. The majority of the land cover in the Adirondacks is forested with 47% of the total area deciduous, 20% coniferous and 10% mixed. We used litterfall plus throughfall deposition as the total atmospheric Hg deposition to coniferous and deciduous forests during the leaf-on period, and wet Hg deposition plus modeled atmospheric dry Hg deposition as the total Hg deposition to the deciduous forest during the leaf-off period and for the non-forested areas year-around. To estimate atmospheric dry Hg deposition we used the Big Leaf model. The average atmospheric Hg deposition to the Adirondacks was estimated as 17.4 [Formula: see text]g m[Formula: see text] yr[Formula: see text] with a range of -3.7-46.0 [Formula: see text]g m[Formula: see text] yr[Formula: see text]. Atmospheric Hg dry deposition (370 kg yr[Formula: see text]) was found to be more important than wet deposition (210 kg yr[Formula: see text]) to the entire Adirondacks (2.4 million ha). The spatial pattern showed a large variation in atmospheric Hg deposition with scattered areas in the eastern Adirondacks having total Hg deposition greater than 30 ?g m(-2) yr(-1), while the southwestern and the northern areas received Hg deposition ranging from 25-30 ?g m(-2) yr(-1).
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Project description:Mercury (Hg), a neurotoxic heavy metal, is transferred to marine and terrestrial ecosystems through atmospheric transport. Recent studies have highlighted the role of vegetation uptake as a sink for atmospheric elemental mercury (Hg0) and a source of Hg to soils. However, the global magnitude of the Hg0 vegetation uptake flux is highly uncertain, with estimates ranging 1000-4000 Mg per year. To constrain this sink, we compare simulations in the chemical transport model GEOS-Chem with a compiled database of litterfall, throughfall, and flux tower measurements from 93 forested sites. The prior version of GEOS-Chem predicts median Hg0 dry deposition velocities similar to litterfall measurements from Northern hemisphere temperate and boreal forests (∼0.03 cm s-1), yet it underestimates measurements from a flux tower study (0.04 cm s-1vs. 0.07 cm s-1) and Amazon litterfall (0.05 cm s-1vs. 0.17 cm s-1). After revising the Hg0 reactivity within the dry deposition parametrization to match flux tower and Amazon measurements, GEOS-Chem displays improved agreement with the seasonality of atmospheric Hg0 observations in the Northern midlatitudes. Additionally, the modelled bias in Hg0 concentrations in South America decreases from +0.21 ng m-3 to +0.05 ng m-3. We calculate a global flux of Hg0 dry deposition to land of 2276 Mg per year, approximately double previous model estimates. The Amazon rainforest contributes 29% of the total Hg0 land sink, yet continued deforestation and climate change threatens the rainforest's stability and thus its role as an important Hg sink. In an illustrative worst-case scenario where the Amazon is completely converted to savannah, GEOS-Chem predicts that an additional 283 Mg Hg per year would deposit to the ocean, where it can bioaccumulate in the marine food chain. Biosphere-atmosphere interactions thus play a crucial role in global Hg cycling and should be considered in assessments of future Hg pollution.
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Project description:Human activities have increased the global circulation of mercury, a potent neurotoxin. Mercury can be converted into methylmercury, which biomagnifies along aquatic food chains and leads to high exposure in fish-eating populations. Here we quantify temporal trends in the ocean-to-land transport of total mercury and methylmercury from fisheries and we estimate potential human mercury intake through fish consumption in 175 countries. Mercury export from the ocean increased over time as a function of fishing pressure, especially on upper-trophic-level organisms. In 2014, over 13 metric tonnes of mercury were exported from the ocean. Asian countries were important contributors of mercury export in the last decades and the western Pacific Ocean was identified as the main source. Estimates of per capita mercury exposure through fish consumption showed that populations in 38% of the 175 countries assessed, mainly insular and developing nations, were exposed to doses of methylmercury above governmental thresholds. Our study shows temporal trends and spatial patterns of Hg transport by fisheries. Given the high mercury intake through seafood consumption observed in several understudied yet vulnerable coastal communities, we recommend a comprehensive assessment of the health exposure risk of those populations.
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Project description:As global climate continues to warm, melting of glaciers releases a large quantity of mercury (Hg) originally locked in ice into the atmosphere and downstream ecosystems. Here, we show an opposite process that captures atmospheric Hg through glacier-to-vegetation succession. Our study using stable isotope techniques at 3 succession sites on the Tibetan Plateau reveals that evolving vegetation serves as an active "pump" to take up gaseous elemental mercury (Hg0) from the atmosphere. The accelerated uptake enriches the Hg pool size in glacier-retreated areas by a factor of ∼10 compared with the original pool size in the glacier. Through an assessment of Hg source-sink relationship observed in documented glacier-retreated areas in the world (7 sites of tundra/steppe succession and 5 sites of forest succession), we estimate that 400 to 600 Mg of Hg has been accumulated in glacier-retreated areas (5‰ of the global land surface) since the Little Ice Age (∼1850). By 2100, an additional ∼300 Mg of Hg will be sequestered from the atmosphere in glacier-retreated regions globally, which is ∼3 times the total Hg mass loss by meltwater efflux (∼95 Mg) in alpine and subpolar glacier regions. The recapturing of atmospheric Hg by vegetation in glacier-retreated areas is not accounted for in current global Hg models. Similar processes are likely to occur in other regions that experience increased vegetation due to climate or land use changes, which need to be considered in the assessment of global Hg cycling.
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