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Mercury is a toxic environmental pollutant emitted into the atmosphere by both natural and anthropogenic sources. In Australia, previous estimates of anthropogenic mercury emissions differ by up to a factor of three, with existing inventories either outdated or inaccurate and several lacking Australia-specific input data. Here, we develop a twenty-year inventory of Australian anthropogenic mercury emissions spanning 2000-2019 with annual resolution. Our inventory uses Australia-specific data where possible and incorporates processes not included in other Australian inventories, such as delayed release effects from waste emissions. We show that Australian anthropogenic mercury emissions have decreased by more than a factor of two over the past twenty years, with the largest decrease from the gold production sector followed by brown coal-fired power plants and commercial product waste. Only the aluminium sector has shown a notable increase in mercury emissions. Using a global 3-D chemical transport model (GEOS-Chem), we show that the reduction in emissions has led to a small decrease in mercury deposition to the Australian continent, with annual oxidised mercury deposition ∼3-4% lower with present day emissions than with emissions from the year 2000. We also find that Australian emissions are not accurately represented in recent global emissions inventories and that differences between inventories have a larger impact than emissions trends on simulated mercury deposition. Overall, this work suggests a significant benefit to Australia from the Minamata Convention, with further reductions to Australian mercury deposition expected from decreases in both Australian and global anthropogenic emissions.

Mercury (Hg) is a naturally occurring element in the Earth's crust. It can be harmful to human health when released in large quantities and/or converted to the neurotoxicant methyl mercury in aquatic ecosystems. This study analyzes global and regional trends in anthropogenic Hg releases to the atmosphere between 2010 and 2015, as well as the associated trends in modeled and measured Hg concentrations at sites around the world. In general, we find that global Hg emissions and concentrations have grown slightly in this period, as declines from the phase-out of commercial Hg use in the developed world have been more than matched by increases in Hg-related activities in the industrializing countries of the world. We estimate that global Hg emissions between 2010 and 2015 have grown at a rate of 1.8%/yr, from 2188 Mg (+44%/-20%, 80% C.I.) in 2010 to 2390 Mg (+42%/-19%, 80% C.I.) in 2015. Regionally, emissions declined over this period in the U.S. (−10%), OECD Europe (−5.8%), and Canada (−3.2%), while they increased in Central America (+5.4%), South Asia (+4.6%), and Eastern Africa (+4.0%). East Asia remained the largest emitting region at 1012 Mg in 2015, though growth there has slowed significantly in recent years. The production of Hg (+7.9%), caustic soda (+6.3%), and cement (+6.3%) showed the highest increases by source type, though artisanal and small-scale gold mining (ASGM) was the single largest source of emissions in 2015 (775 Mg). The commercial use of Hg in dental applications (−5.6%) and electrical equipment (−5.2%) continued to decline. These emission trends show a continuation of the regional and sectoral shifts that began in the 1970s, but with a resulting reversal in global trends, because the benefits from Hg phase-out in North America and Europe have been largely realized and industrial growth in developing countries has begun to dominate. The emission trends are in agreement with trends in modeled and measured concentrations, which show small declines in surface air total gaseous Hg concentrations in eastern North America and Western Europe between 2010 and 2015, but slight increases for much of the rest of the world, driven by the continued increases in emissions from Asia and from ASGM. Our results suggest that reductions of Hg in the North Atlantic region have been largely successful, and focus now needs to shift to Asia and to the continued practice of ASGM worldwide.

The sensitivity of climate models to the characterization of African aerosol particles is poorly understood. Africa is a major source of dust and biomass burning aerosols and this represents an important research gap in understanding the impact of aerosols on radiative forcing of the climate system. Here we evaluate the current representation of aerosol particles in the Conformal Cubic Atmospheric Model (CCAM) with ground-based remote retrievals across Africa, and additionally provide an analysis of observed aerosol optical depth at 550 nm (AOD550 nm) and Ångström exponent data from 34 Aerosol Robotic Network (AERONET) sites. Analysis of the 34 long-term AERONET sites confirms the importance of dust and biomass burning emissions to the seasonal cycle and magnitude of AOD550 nm across the continent and the transport of these emissions to regions outside of the continent. In general, CCAM captures the seasonality of the AERONET data across the continent. The magnitude of modeled and observed multiyear monthly average AOD550 nm overlap within ±1 standard deviation of each other for at least 7 months at all sites except the Réunion St Denis Island site (Réunion St. Denis). The timing of modeled peak AOD550 nm in southern Africa occurs 1 month prior to the observed peak, which does not align with the timing of maximum fire counts in the region. For the western and northern African sites, it is evident that CCAM currently overestimates dust in some regions while others (e.g., the Arabian Peninsula) are better characterized. This may be due to overestimated dust lifetime, or that the characterization of the soil for these areas needs to be updated with local information. The CCAM simulated AOD550 nm for the global domain is within the spread of previously published results from CMIP5 and AeroCom experiments for black carbon, organic carbon, and sulfate aerosols. The model's performance provides confidence for using the model to estimate large-scale regional impacts of African aerosols on radiative forcing, but local feedbacks between dust aerosols and climate over northern Africa and the Mediterranean may be overestimated.

We estimate that a cumulative total of 1540 (1060–2800) Gg (gigagrams, 109 grams or thousand tonnes) of mercury (Hg) have been released by human activities up to 2010, 73% of which was released after 1850. Of this liberated Hg, 470 Gg were emitted directly into the atmosphere, and 74% of the air emissions were elemental Hg. Cumulatively, about 1070 Gg were released to land and water bodies. Though annual releases of Hg have been relatively stable since 1880 at 8 ± 2 Gg, except for wartime, the distributions of those releases among source types, world regions, and environmental media have changed dramatically. Production of Hg accounts for 27% of cumulative Hg releases to the environment, followed by silver production (24%) and chemicals manufacturing (12%). North America (30%), Europe (27%), and Asia (16%) have experienced the largest releases. Biogeochemical modeling shows a 3.2-fold increase in the atmospheric burden relative to 1850 and a contemporary atmospheric reservoir of 4.57 Gg, both of which agr...

Marine cloud brightening (MCB) is proposed to offset global warming by emitting sea salt aerosols to the tropical marine boundary layer, which increases aerosol and cloud albedo. Sea salt aerosol is the main source of tropospheric reactive chlorine (Cly) and bromine (Bry). The effects of additional sea salt on atmospheric chemistry have not been explored. We simulate sea salt aerosol injections for MCB under two scenarios (212–569 Tg/a) in the GEOS‐Chem global chemical transport model, only considering their impacts as a halogen source. Globally, tropospheric Cly and Bry increase (20–40%), leading to decreased ozone (−3 to −6%). Consequently, OH decreases (−3 to −5%), which increases the methane lifetime (3–6%). Our results suggest that the chemistry of the additional sea salt leads to minor total radiative forcing compared to that of the sea salt aerosol itself (~2%) but may have potential implications for surface ozone pollution in tropical coastal regions., Key Points Sea salt aerosol emissions for Marine Cloud Brightening geoengineering are implemented in a global chemical transport modelThis leads to changes in global tropospheric Bry and Cly (+20 to 40%), ozone (−3 to −6%), OH (−2 to −4%), and methane lifetime (+3 to 6%)Chemistry of the added sea salt leads to minor total radiative forcing (−20 to −50 mW/m2) but may have implications for ozone pollution

Air-sea exchange of mercury (Hg) is the largest flux between Earth system reservoirs. Global models simulate air-sea exchange based either on an atmospheric or ocean model simulation and treat the other media as a boundary condition. Here we develop a new modeling capability (NJUCPL) that couples GEOS-Chem (atmospheric model) and MITgcm (ocean model) at the native hourly model time step. The coupled model is evaluated against high-frequency simultaneous measurements of elemental mercury (Hg

Atmospheric mercury (Hg) in the Arctic shows much weaker or insignificant annual declines relative to northern midlatitudes over the past decade (2000-2009) but with strong seasonality in trends. W ...

Centuries of anthropogenic releases have releases in a global legacy of mercury (Hg) contamination. Here we use a global model to quantify the impact of uncertainty in Hg atmospheric emissions and cycling -On anthropogenic enrichment and discuss implications for future Hg levels. The plausibility of sensitivity simulations is evaluated against multiple independent lines of Observation, including natural archives and direct measurements of present-day environmental Hg concentrations. It has been previously reported that pre-industriaVenrichment recorded in sediment and peat disagree by more than a factor of 10. We find this difference is largely erroneous and caused by comparing peat and sediment against different reference time periods. After correcting this inconsistenr-yi, median enrichment in Hg accumulation since pre-industrial 1760 to 1880 is a factor of 4.3 for peat and 3.0 for sediment. Pre-industrial accumulation in peat and sediment is a factor of greater than the precolonial era (3000-BC to 1550 AD). Model scenarios that omit atmospheric emissions of Hg,froin early mining are inconsistent with observational constraints on the present-day atmospheric, oceanic, and soil Hg reservoirs, as well as the magnitude of enrichment in archives. Future reductions in anthropogenic emissions will initiate a decline in atmospheric concentrations within 1 year, but stabilization of subsurface and deep oaearr Hg levels requires aggressive controls. These findings are robust to the ranges of uncertainty in past emissions arid Hg cycling.

The sensitivity of climate models to the characterization of African aerosol particles is poorly understood. Africa is a major source of dust and biomass burning aerosols and so this represents an important research gap in understanding the impact of aerosols on radiative forcing of the climate system. Here we evaluate the current representation of aerosol particles in the Conformal Cubic Atmospheric Model (CCAM) with ground-based observations across Africa, and additionally provide an analysis of aerosol optical depth at 550 nm (AOD550nm) and Ångström exponent data from thirty-four Aerosol Robotic Network (AERONET) sites. Analysis of the 34 long-term AERONET sites confirms the importance of dust and biomass burning emissions to the seasonal cycle and magnitude of AOD550nm across the continent and the transport of these emissions to regions outside of the continent. Western African sites had the largest AOD550nm values, on average, with the timing and magnitude of AOD550nm maxima dominated by desert dust. The impact of dust on aerosol loading is also apparent at northern African sites, with peak AOD550nm occurring later than the western sites. The seasonal variation in the location of the intertropical convergence zone and associated northward shift in dust transport may be responsible for the shift in timing of maximum AOD550nm between the western and northern African sites. Southern African sites have the lowest AOD550nm values on average, and peak during the biomass burning period. The outflow of these aerosol particles was observed at Ascension Island and Reunion Island AERONET stations. In general, CCAM captures well the seasonality of the AERONET data across the continent. The magnitude of modeled and observed multi-year monthly average AOD550nm overlap within ±1 standard deviation of each other for at least 7 months at all sites except Reunion Island. The timing of peak AOD550nm in southern Africa in the model occurs one month prior to the observed peak, which does not align with the timing of maximum fire counts in the region. For the western and northern African sites, it is evident that CCAM currently overestimates dust in some regions while others (e.g., the Arabian Peninsula) are better characterized. This may be due to overestimated dust lifetime, or that the characterization of the soil for these areas needs to be updated with local information. The CCAM simulated AOD550nm for the global domain is within the spread of previously published results from CMIP5 and AeroCom experiments for black carbon, organic carbon and sulfate aerosols. The model’s performance provides confidence for using the model to estimate large-scale regional impacts of African aerosols on radiative forcing, but local feedbacks between dust aerosols and climate over northern Africa and the Mediterranean may be overestimated.

Mercury (Hg) is emitted to the atmosphere mainly as volatile elemental Hg0. Oxidation to water-soluble HgII controls Hg deposition to ecosystems. Here we implement a new mechanism for atmospheric Hg0 / HgII redox chemistry in the GEOS-Chem global model and examine the implications for the global atmospheric Hg budget and deposition patterns. Our simulation includes a new coupling of GEOS-Chem to an ocean general circulation model (MITgcm), enabling a global 3-D representation of atmosphere-ocean Hg0 / HgII cycling. We find that atomic bromine (Br) of marine organobromine origin is the main atmospheric Hg0 oxidant, and that second-stage HgBr oxidation is mainly by the NO2 and HO2 radicals. The resulting lifetime of tropospheric Hg0 against oxidation is 2.7 months, shorter than in previous models. Fast HgII atmospheric reduction must occur in order to match the ~ 6-month lifetime of Hg against deposition implied by the observed atmospheric variability of total gaseous mercury (TGM ≡ Hg0 + HgII(g)). We implement this reduction in GEOS-Chem as photolysis of aqueous-phase HgII-organic complexes in aerosols and clouds, resulting in a TGM lifetime of 5.2 months against deposition and matching both mean observed TGM and its variability. Model sensitivity analysis shows that the interhemispheric gradient of TGM, previously used to infer a longer Hg lifetime against deposition, is misleading because southern hemisphere Hg mainly originates from oceanic emissions rather than transport from the northern hemisphere. The model reproduces the observed seasonal TGM variation at northern mid-latitudes (maximum in February, minimum in September) driven by chemistry and oceanic evasion, but does not reproduce the lack of seasonality observed at southern hemisphere marine sites. Aircraft observations in the lowermost stratosphere show a strong TGM-ozone relationship indicative of fast Hg0 oxidation, but we show that this relationship provides only a weak test of Hg chemistry because it is also influenced by mixing. The model reproduces observed Hg wet deposition fluxes over North America, Europe, and China, including the maximum over the US Gulf Coast driven by HgBr oxidation by NO2 and HO2. Low Hg wet deposition observed over rural China is attributed to fast HgII reduction in the presence of high organic aerosol concentrations. We find that 80 % of global HgII deposition takes place over the oceans, reflecting the marine origin of Br and low concentrations of marine organics for HgII reduction, and most of HO2 and NO2 for second-stage HgBr oxidation.

When released to the biosphere, mercury (Hg) is very mobile and can take millennia to be returned to a secure, long-term repository. Understanding where and when Hg was released as a result of human activities allows better quantification of present-day reemissions and future trajectories of environmental concentrations. In this work, we estimate the time-varying releases of Hg in seven world regions over the 500 year period, 1510–2010. By our estimation, this comprises 95% of all-time anthropogenic releases. Globally, 1.47 Tg of Hg were released in this period, 23% directly to the atmosphere and 77% to land and water bodies. Cumulative releases have been largest in Europe (427 Gg) and North America (413 Gg). In some world regions (Africa/Middle East and Oceania), almost all (>99%) of the Hg is relatively recent (emitted since 1850), whereas in South America it is mostly of older vintage (63% emitted before 1850). Asia was the greatest-emitting region in 2010, while releases in Europe and North America have declined since the 1970s, as recognition of the risks posed by Hg have led to its phase-out in commercial usage. The continued use of Hg in artisanal and small-scale gold mining means that the Africa/Middle East region is now a major contributor. We estimate that 72% of cumulative Hg emissions to air has been in the form of elemental mercury (Hg0), which has a long lifetime in the atmosphere and can therefore be transported long distances. Our results show that 83% of the total Hg has been released to local water bodies, onto land, or quickly deposited from the air in divalent (HgII) form. Regionally, this value ranges from 77% in Africa/Middle East and Oceania to 89% in South America. Results from global biogeochemical modeling indicate improved agreement of the refined emission estimates in this study with archival records of Hg accumulation in estuarine and deep ocean sediment.

Aircraft and satellite observations indicate the presence of ppt (pptpmol/mol) levels of BrO in the free troposphere with important implications for the tropospheric budgets of ozone, OH, and mercury. We can reproduce these observations with the GEOS-Chem global tropospheric chemistry model by including a broader consideration of multiphase halogen (Br-Cl) chemistry than has been done in the past. Important reactions for regenerating BrO from its nonradical reservoirs include HOBr+Br-/Cl- in both aerosols and clouds, and oxidation of Br- by ClNO3 and ozone. Most tropospheric BrO in the model is in the free troposphere, consistent with observations and originates mainly from the photolysis and oxidation of ocean-emitted CHBr3. Stratospheric input is also important in the upper troposphere. Including production of gas phase inorganic bromine from debromination of acidified sea salt aerosol increases free tropospheric Br-y by about 30%. We find HOBr to be the dominant gas-phase reservoir of inorganic bromine. Halogen (Br-Cl) radical chemistry as implemented here in GEOS-Chem drives 14% and 11% decreases in the global burdens of tropospheric ozone and OH, respectively, a 16% increase in the atmospheric lifetime of methane, and an atmospheric lifetime of 6months for elemental mercury. The dominant mechanism for the Br-Cl driven tropospheric ozone decrease is oxidation of NOx by formation and hydrolysis of BrNO3 and ClNO3.

Observations of elemental mercury (Hg(0)) at sites in North America and Europe show large decreases (∼ 1-2% y(-1)) from 1990 to present. Observations in background northern hemisphere air, including Mauna Loa Observatory (Hawaii) and CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) aircraft flights, show weaker decreases (

Mercury (Hg) stable isotopes provide a new tool to trace the biogeochemical cycle of Hg. An inventory of the isotopic composition of historical anthropogenic Hg emissions is important to understand sources and post-emission transformations of Hg. We build on existing global inventories of anthropogenic Hg emissions to the atmosphere to develop the first corresponding historical Hg isotope inventories for total Hg (THg) and three Hg species: gaseous elemental Hg (GEM), gaseous oxidized Hg (GOM) and particulate-bound Hg (PBM). We compile δ202Hg and Δ199Hg of major Hg emissions source materials. Where possible, δ202Hg and Δ199Hg values in emissions are corrected for the mass dependent Hg isotope fractionation during industrial processing. The framework and Hg isotope inventories can be updated and improved as new data become available. Simulated THg emissions from all sectors between 1850s and 2010s generally show an increasing trend (−1.1‰ to −0.7‰) for δ202Hg, and a stable trend (−0.02‰ to −0.04‰) for Δ199Hg. Δ200Hg are near-zero in source materials and therefore emissions. The δ202Hg trend generally reflects a shift of historically dominant Hg emissions from 19th century Hg mining and liquid Hg0 uses in Au/Ag refining to 20th century coal combustion and non-ferrous metal production. The historical δ202Hg and Δ199Hg curves of GEM closely follow those of THg. The δ202Hg curves of GOM and PBM show no trends. Δ199Hg values for both GOM and PBM decrease from the 1850s to 1950s by ∼0.1‰, and then gradually rebound towards the 2010s. Our updated δ202Hg values (−0.76 ± 0.11 ‰, 1SD, n=9) of bulk emissions from passively degassing volcanoes overlap with δ202Hg of present-day anthropogenic THg emissions.

The intentional use of mercury (Hg) in products and processes ("commercial Hg") has contributed a large and previously unquantified anthropogenic source of Hg to the global environment over the industrial era, with major implications for Hg accumulation in environmental reservoirs. We present a global inventory of commercial Hg uses and releases to the atmosphere, water, soil, and landfills from 1850 to 2010. Previous inventories of anthropogenic Hg releases have focused almost exclusively on atmospheric emissions from "byproduct" sectors (e.g., fossil fuel combustion). Cumulative anthropogenic atmospheric Hg emissions since 1850 have recently been estimated at 215 Gg (only including commercial Hg releases from chlor-alkali production, waste incineration, and mining). We find that other commercial Hg uses and nonatmospheric releases from chlor-alkali and mining result in an additional 540 Gg of Hg released to the global environment since 1850 (air: 20%; water: 30%; soil: 30%; landfills: 20%). Some of this release has been sequestered in landfills and benthic sediments, but 310 Gg actively cycles among geochemical reservoirs and contributes to elevated present-day environmental Hg concentrations. Commercial Hg use peaked in 1970 and has declined sharply since. We use our inventory of historical environmental releases to force a global biogeochemical model that includes new estimates of the global burial in ocean margin sediments. Accounting for commercial Hg releases improves model consistency with observed atmospheric concentrations and associated historical trends.

Rivers are an important source of mercury (Hg) to marine ecosystems. Based on an analysis of compiled observations, we estimate global present-day Hg discharges from rivers to ocean margins are 27 ± 13 Mmol a(-1) (5500 ± 2700 Mg a(-1)), of which 28% reaches the open ocean and the rest is deposited to ocean margin sediments. Globally, the source of Hg to the open ocean from rivers amounts to 30% of atmospheric inputs. This is larger than previously estimated due to accounting for elevated concentrations in Asian rivers and variability in offshore transport across different types of estuaries. Riverine inputs of Hg to the North Atlantic have decreased several-fold since the 1970s while inputs to the North Pacific have increased. These trends have large effects on Hg concentrations at ocean margins but are too small in the open ocean to explain observed declines of seawater concentrations in the North Atlantic or increases in the North Pacific. Burial of Hg in ocean margin sediments represents a major sink in the global Hg biogeochemical cycle that has not been previously considered. We find that including this sink in a fully coupled global biogeochemical box model helps to balance the large anthropogenic release of Hg from commercial products recently added to global inventories. It also implies that legacy anthropogenic Hg can be removed from active environmental cycling on a faster time scale (centuries instead of millennia). Natural environmental Hg levels are lower than previously estimated, implying a relatively larger impact from human activity.