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Past and present anthropogenic mercury (Hg) release to ecosystems causes neurotoxicity and cardiovascular disease in humans with an estimated economic cost of $117 billion USD annually. Humans are primarily exposed to Hg via the consumption of contaminated freshwater and marine fish. The UNEP Minamata Convention on Hg aims to curb Hg release to the environment and is accompanied by global Hg monitoring efforts to track its success. The biogeochemical Hg cycle is a complex cascade of release, dispersal, transformation and bio-uptake processes that link Hg sources to Hg exposure. Global change interacts with the Hg cycle by impacting the physical, biogeochemical and ecological factors that control these processes. In this review we examine how global change such as biome shifts, deforestation, permafrost thaw or ocean stratification will alter Hg cycling and exposure. Based on past declines in Hg release and environmental levels, we expect that future policy impacts should be distinguishable from global change effects at the regional and global scales.

 

Terrestrial volcanism is known to emit mercury (Hg) into the atmosphere. However, despite many years of investigation, its net impact on the atmospheric Hg budget remains insufficiently constrained, in part because the transformations of Hg in volcanic plumes as they age and mix with background air are poorly understood. Here we report the observation of complete gaseous elemental mercury (GEM) depletion events in dilute and moderately aged (∼3–7 hours) volcanic plumes from Piton de la Fournaise on Réunion Island. While it has been suggested that co-emitted bromine could, once photochemically activated, deplete GEM in a volcanic plume, we measured low bromine concentrations in both the gas- and particle-phase and observed complete GEM depletion even before sunrise, ruling out a leading role of bromine chemistry here. Instead, we hypothesize that the GEM depletions were mainly caused by gas–particle interactions with sulfate-rich volcanic particles (mostly of submicron size), abundantly present in the dilute plume. We consider heterogeneous GEM oxidation and GEM uptake by particles as plausible manifestations of such a process and derive empirical rate constants. By extrapolation, we estimate that volcanic aerosols may scavenge 210 Mg y−1 (67–480 Mg y−1) of Hg from the atmosphere globally, acting effectively as atmospheric mercury sink. While this estimate is subject to large uncertainties, it highlights that Hg transformations in aging volcanic plumes must be better understood to determine the net impact of volcanism on the atmospheric Hg budget and Hg deposition pathways. 

The driving forces, kill and recovery mechanisms for the end-Permian mass extinction (EPME), the largest Phanerozoic biological crisis, are under debate. Sedimentary records of mercury enrichment and mercury isotopes have suggested the impact of volcanism on the EPME, yet the causes of mercury enrichment and isotope variations remain controversial. Here, we model mercury isotope variations across the EPME to quantitatively assess the effects of volcanism, terrestrial erosion and photic zone euxinia (PZE, toxic, sulfide-rich conditions). Our numerical model shows that while large-scale volcanism remains the main driver of widespread mercury enrichment, the negative shifts of Δ¹⁹⁹Hg isotope signature across the EPME cannot be fully explained by volcanism or terrestrial erosion as proposed before, but require additional fractionation by marine mercury photoreduction under enhanced PZE conditions. Thus our model provides further evidence for widespread and prolonged PZE as a key kill mechanism for both the EPME and the impeded recovery afterward.

 

Abstract. The tundra plays a pivotal role in the Arctic mercury(Hg) cycle by storing atmospheric Hg deposition and shuttling it to theArctic Ocean. A recent study revealed that 70 % of the atmospheric Hgdeposition to the tundra occurs through gaseous elemental mercury (GEM or Hg(0))uptake by vegetation and soils. Processes controlling land–atmosphereexchange of Hg(0) in the Arctic tundra are central, but remainunderstudied. Here, we combine Hg stable isotope analysis of Hg(0) in theatmosphere, interstitial snow air, and soil pore air, with Hg(0) fluxmeasurements in a tundra ecosystem at Toolik Field Station in northernAlaska (USA). In the dark winter months, planetary boundary layer (PBL)conditions and Hg(0) concentrations were generally stable throughout the dayand small Hg(0) net deposition occurred. In spring, halogen-inducedatmospheric mercury depletion events (AMDEs) occurred, with the fastre-emission of Hg(0) after AMDEs resulting in net emission fluxes of Hg(0).During the short snow-free growing season in summer, vegetation uptake ofatmospheric Hg(0) enhanced atmospheric Hg(0) net deposition to the Arctictundra. At night, when PBL conditions were stable, ecosystem uptake ofatmospheric Hg(0) led to a depletion of atmospheric Hg(0). The night-timedecline of atmospheric Hg(0) was concomitant with a depletion of lighterHg(0) isotopes in the atmospheric Hg pool. The enrichment factor,ε202Hgvegetationuptake=-4.2 ‰ (±1.0 ‰) was consistentwith the preferential uptake of light Hg(0) isotopes by vegetation. Hg(0)flux measurements indicated a partial re-emission of Hg(0) during daytime,when solar radiation was strongest. Hg(0) concentrations in soil pore airwere depleted relative to atmospheric Hg(0) concentrations, concomitant withan enrichment of lighter Hg(0) isotopes in the soil pore air, ε202Hgsoilair-atmosphere=-1.00 ‰(±0.25 ‰) and E199Hgsoilair-atmosphere=0.07 ‰ (±0.04 ‰). Thesefirst Hg stable isotope measurements of Hg(0) in soil pore air areconsistent with the fractionation previously observed during Hg(0) oxidationby natural humic acids, suggesting abiotic oxidation as a cause for observedsoil Hg(0) uptake. The combination of Hg stable isotope fingerprints withHg(0) flux measurements and PBL stability assessment confirmed a dominantrole of Hg(0) uptake by vegetation in the terrestrial–atmosphere exchange ofHg(0) in the Arctic tundra. 

A major surface circulation feature of the Arctic Ocean is the Transpolar Drift (TPD), a current that transports river‐influenced shelf water from the Laptev and East Siberian Seas toward the center of the basin and Fram Strait. In 2015, the international GEOTRACES program included a high‐resolution pan‐Arctic survey of carbon, nutrients, and a suite of trace elements and isotopes (TEIs). The cruises bisected the TPD at two locations in the central basin, which were defined by maxima in meteoric water and dissolved organic carbon concentrations that spanned 600 km horizontally and ~25–50 m vertically. Dissolved TEIs such as Fe, Co, Ni, Cu, Hg, Nd, and Th, which are generally particle‐reactive but can be complexed by organic matter, were observed at concentrations much higher than expected for the open ocean setting. Other trace element concentrations such as Al, V, Ga, and Pb were lower than expected due to scavenging over the productive East Siberian and Laptev shelf seas. Using a combination of radionuclide tracers and ice drift modeling, the transport rate for the core of the TPD was estimated at 0.9 ± 0.4 Sv (10⁶ m³ s⁻¹). This rate was used to derive the mass flux for TEIs that were enriched in the TPD, revealing the importance of lateral transport in supplying materials beneath the ice to the central Arctic Ocean and potentially to the North Atlantic Ocean via Fram Strait. Continued intensification of the Arctic hydrologic cycle and permafrost degradation will likely lead to an increase in the flux of TEIs into the Arctic Ocean.