10 research outputs found
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Historical Mercury Releases from Commercial Products: Global Environmental Implications
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.Engineering and Applied Science
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An Improved Global Model for Air-Sea Exchange of Mercury: High Concentrations over the North Atlantic
We develop an improved treatment of the surface ocean in the GEOS-Chem global 3-D biogeochemical model for mercury (Hg). We replace the globally uniform subsurface ocean Hg concentrations used in the original model with basin-specific values based on measurements. Updated chemical mechanisms for Hg0/HgII redox reactions in the surface ocean include both photochemical and biological processes, and we improved the parametrization of particle-associated Hg scavenging. Modeled aqueous Hg concentrations are consistent with limited surface water observations. Results more accurately reproduce high-observed MBL concentrations over the North Atlantic (NA) and the associated seasonal trends. High seasonal evasion in the NA is driven by inputs from Hg enriched subsurface waters through entrainment and Ekman pumping. Globally, subsurface waters account for 40% of Hg inputs to the ocean mixed layer, and 60% is from atmospheric deposition. Although globally the ocean is a net sink for 3.8 Mmol Hg y−1, the NA is a net source to the atmosphere, potentially due to enrichment of subsurface waters with legacy Hg from historical anthropogenic sources.Engineering and Applied Science
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Source Attribution of Poly- and Perfluoroalkyl Substances (PFASs) in Surface Waters from Rhode Island and the New York Metropolitan Area
Exposure to poly- and perfluoroalkyl substances (PFASs) has been associated with adverse health effects in humans and wildlife. Understanding pollution sources is essential for environmental regulation, but source attribution for PFASs has been confounded by limited information about industrial releases and rapid changes in chemical production. Here we use principal component analysis (PCA), hierarchical clustering, and geospatial analysis to understand source contributions to 14 PFASs measured across 37 sites in the northeastern United States in 2014. PFASs are significantly elevated in urban areas compared to rural sites except for perfluorobutanesulfonate, N-methyl perfluorooctanesulfonamidoacetic acid, perfluoroundecanate, and perfluorododecanate. The highest PFAS concentrations across sites were those of perfluorooctanate (PFOA, 56 ng L−1) and perfluorohexanesulfonate (PFHxS, 43 ng L−1), and perfluorooctanesulfonate (PFOS) levels are lower than earlier measurements of U.S. surface waters. PCA and cluster analysis indicate three main statistical groupings of PFASs. Geospatial analysis of watersheds reveals the first component/cluster originates from a mixture of contemporary point sources such as airports and textile mills. Atmospheric sources from the waste sector are consistent with the second component, and the metal smelting industry plausibly explains the third component. We find this source-attribution technique is effective for better understanding PFAS sources in urban areas.Engineering and Applied Science
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Gas-Particle Partitioning of Atmospheric Hg(II) and Its Effect on Global Mercury Deposition
Atmospheric deposition of Hg(II) represents a major input of mercury to surface environments. The phase of Hg(II) (gas or particle) has important implications for deposition. We use long-term observations of reactive gaseous mercury (RGM, the gaseous component of Hg(II)), particle-bound mercury (PBM, the particulate component of Hg(II)), fine particulate matter (PM2.5), and temperature (T) at five sites in North America to derive an empirical gas-particle partitioning relationship log10(K−1) = (10±1)–(2500±300)/T where K = (PBM/PM2.5)/RGM with PBM and RGM in common mixing ratio units, PM2.5 in μg m−3, and T in K. This relationship is within the range of previous work but is based on far more extensive data from multiple sites. We implement this empirical relationship in the GEOS-Chem global 3-D Hg model to partition Hg(II) between the gas and particle phases. The resulting gas-phase fraction of Hg(II) ranges from over 90 % in warm air with little aerosol to less than 10 % in cold air with high aerosol. Hg deposition to high latitudes increases because of more efficient scavenging of particulate Hg(II) by precipitating snow. Model comparison to Hg observations at the North American surface sites suggests that subsidence from the free troposphere (warm air, low aerosol) is a major factor driving the seasonality of RGM, while elevated PBM is mostly associated with high aerosol loads. Simulation of RGM and PBM at these sites is improved by including fast in-plume reduction of Hg(II) emitted from coal combustion and by assuming that anthropogenic particulate Hg(p) behaves as semi-volatile Hg(II) rather than as a refractory particulate component. We improve the simulation of Hg wet deposition fluxes in the US relative to a previous version of GEOS-Chem; this largely reflects independent improvement of the washout algorithm. The observed wintertime minimum in wet deposition fluxes is attributed to inefficient snow scavenging of gas-phase Hg(II).Earth and Planetary SciencesEngineering and Applied Science
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Global Source–Receptor Relationships for Mercury Deposition Under Present-Day and 2050 Emissions Scenarios
Global policies regulating anthropogenic mercury require an understanding of the relationship between emitted and deposited mercury on intercontinental scales. Here, we examine source–receptor relationships for present-day conditions and four 2050 IPCC scenarios encompassing a range of economic development and environmental regulation projections. We use the GEOS-Chem global model to track mercury from its point of emission through rapid cycling in surface ocean and land reservoirs to its accumulation in longer lived ocean and soil pools. Deposited mercury has a local component (emitted HgII, lifetime of 3.7 days against deposition) and a global component (emitted Hg0, lifetime of 6 months against deposition). Fast recycling of deposited mercury through photoreduction of HgII and re-emission of Hg0 from surface reservoirs (ice, land, surface ocean) increases the effective lifetime of anthropogenic mercury to 9 months against loss to legacy reservoirs (soil pools and the subsurface ocean). This lifetime is still sufficiently short that source–receptor relationships have a strong hemispheric signature. Asian emissions are the largest source of anthropogenic deposition to all ocean basins, though there is also regional source influence from upwind continents. Current anthropogenic emissions account for only about one-third of mercury deposition to the global ocean with the remainder from natural and legacy sources. However, controls on anthropogenic emissions would have the added benefit of reducing the legacy mercury re-emitted to the atmosphere. Better understanding is needed of the time scales for transfer of mercury from active pools to stable geochemical reservoirs.Engineering and Applied Science
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Biogeochemical drivers of the fate of riverine mercury discharged to the global and Arctic oceans
Rivers discharge 28 ± 13 Mmol yr1 of mercury (Hg) to ocean margins, an amount comparable to atmospheric deposition to the global oceans. Most of the Hg discharged by rivers is sequestered by burial of benthic sediment in estuaries or the coastal zone, but some is evaded to the atmosphere and some is exported to the open ocean. We investigate the fate of riverine Hg by developing a new global 3-D simulation for Hg in the Massachusetts Institute of Technology ocean general circulation model. The model includes plankton dynamics and carbon respiration (DARWIN project model) coupled to inorganic Hg chemistry. Results are consistent with observed spatial patterns and magnitudes of surface ocean Hg concentrations. We use observational constraints on seawater Hg concentrations and evasion to infer that most Hg from rivers is sorbed to refractory organic carbon and preferentially buried. Only 6% of Hg discharged by rivers (1.8 Mmol yr1 ) is transported to the open ocean on a global basis. This fraction varies from a low of 2.6% in East Asia due to the barrier imposed by the Korean Peninsula and Japanese archipelago, up to 25% in eastern North America facilitated by the Gulf Stream. In the Arctic Ocean, low tributary particle loads and efficient degradation of particulate organic carbon by deltaic microbial communities favor a more labile riverine Hg pool. Evasion of Hg to the Arctic atmosphere is indirectly enhanced by heat transport during spring freshet that accelerates sea ice melt and ice rafting. Discharges of 0.23 Mmol Hg yr1 from Arctic rivers can explain the observed summer maximum in the Arctic atmosphere, and this magnitude of releases is consistent with recent observations. Our work indicates that rivers are major contributors to Hg loads in the Arctic Ocean.Engineering and Applied Science
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Elemental Mercury Concentrations and Fluxes in the Tropical Atmosphere and Ocean
Air–sea exchange of elemental mercury (Hg0) is a critical component of the global biogeochemical Hg cycle. To better understand variability in atmospheric and oceanic Hg0, we collected high-resolution measurements across large gradients in seawater temperature, salinity, and productivity in the Pacific Ocean (20°N-15°S). We modeled surface ocean Hg inputs and losses using an ocean general circulation model (MITgcm) and an atmospheric chemical transport model (GEOS-Chem). Observed surface seawater Hg0 was much more variable than atmospheric concentrations. Peak seawater Hg0 concentrations (∼130 fM) observed in the Pacific intertropical convergence zone (ITCZ) were ∼3-fold greater than surrounding areas (∼50 fM). This is similar to observations from the Atlantic Ocean. Peak evasion in the northern Pacific ITCZ was four times higher than surrounding regions and located at the intersection of high wind speeds and elevated seawater Hg0. Modeling results show that high Hg inputs from enhanced precipitation in the ITCZ combined with the shallow ocean mixed layer in this region drive elevated seawater Hg0 concentrations. Modeled seawater Hg0 concentrations reproduce observed peaks in the ITCZ of both the Atlantic and Pacific Oceans but underestimate its magnitude, likely due to insufficient deep convective scavenging of oxidized Hg from the upper troposphere. Our results demonstrate the importance of scavenging of reactive mercury in the upper atmosphere driving variability in seawater Hg0 and net Hg inputs to biologically productive regions of the tropical ocean.Engineering and Applied Science
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Observed decrease in atmospheric mercury explained by global decline in anthropogenic emissions
Anthropogenic mercury poses risks to humans and ecosystems when converted to methylmercury. A longstanding conundrum has been the apparent disconnect between increasing global emissions trends and measured declines in atmospheric mercury in North America and Europe. This work shows that locally deposited mercury close to coal-fired utilities has declined more rapidly than previously anticipated because of shifts in speciation from air pollution control technology targeted at SO2 and NOx. Reduced emissions from utilities over the past two decades and the phase-out of mercury in many commercial products has led to lower global anthropogenic emissions and associated deposition to ecosystems. This implies that prior policy assessments underestimated the regional benefits of declines in mercury emissions from coal-fired utilities.Engineering and Applied Science
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Global Biogeochemical Implications of Mercury Discharges from Rivers and Sediment Burial
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 plus or minus 13 Mmol a super(-1) (5500 plus or minus 2700 Mg a super(-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.Engineering and Applied Science
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Balancing the benefits of n-3 polyunsaturated fatty acids and the risks of methylmercury exposure from fish consumption
Fish and shellfish are widely available foods that provide important nutrients, particularly n-3 polyunsaturated fatty acids (n-3 PUFAs), to many populations globally. These nutrients, especially docosahexaenoic acid, confer benefits to brain and visual system development in infants and reduce risks of certain forms of heart disease in adults. However, fish and shellfish can also be a major source of methylmercury (MeHg), a known neurotoxicant that is particularly harmful to fetal brain development. This review documents the latest knowledge on the risks and benefits of seafood consumption for perinatal development of infants. It is possible to choose fish species that are both high in n-3 PUFAs and low in MeHg. A framework for providing dietary advice for women of childbearing age on how to maximize the dietary intake of n-3 PUFAs while minimizing MeHg exposures is suggested