The overlooked role of the ocean in mercury cycling in the Arctic (original) (raw)

Methylated Mercury Species in Canadian High Arctic Marine Surface Waters and Snowpacks

Environmental Science & Technology, 2007

We sampled seawater and snowpacks in the Canadian high Arctic for methylated species of mercury (Hg). We discovered that, although seawater sampled under the sea ice had very low concentrations of total Hg (THg, all forms of Hg in a sample; on average 0.14-0.24 ng L -1 ), 30-45% of the THg was in the monomethyl Hg (MMHg) form (on average 0.057-0.095 ng L -1 ), making seawater itself a direct source of MMHg for biomagnification through marine food webs. Seawater under the ice also contained high concentrations of gaseous elemental Hg (GEM; 129 ( 36 pg L -1 ), suggesting that open water regions such as polynyas and ice leads were a net source of ∼130 ( 30 ng Hg m -2 day -1 to the atmosphere. We also found 11.1 ( 4.1 pg L -1 of dimethyl Hg (DMHg) in seawater and calculated that there could be a significant flux of DMHg to the atmosphere from open water regions. This flux could then result in MMHg deposition into nearby snowpacks via oxidation of DMHg to MMHg in the atmosphere. In fact, we found high concentrations of MMHg in a few snowpacks near regions of open water. Interestingly, we discovered a significant log-log relationship between Clconcentrations in snowpacks and concentrations of THg. We hypothesize that as Clconcentrations in snowpacks increase, inorganic Hg(II) occurs principally as less reducible chloro complexes and, hence, remains in an oxidized state. As a result, snowpacks that receive both marine aerosol deposition of Cland deposition of Hg(II) via springtime atmospheric Hg depletion events, for example, may contain significant loads of Hg(II). Overall, though, the median wet/dry loads of Hg in the snowpacks we sampled in the high Arctic (5.2 mg THg ha -1 and 0.03 mg MMHg ha -1 ) were far below wet-only annual THg loadings throughout southern Canada and most of the U.S. (22-200 mg ha -1 ). Therefore, most Arctic snowpacks contribute relatively little to marine pools of both Hg(II) and MMHg at snowmelt.

THE FATE OF MERCURY IN ARCTIC TERRESTRIAL AND AQUATIC ECOSYSTEMS, A REVIEW

Environmental …, 2012

Environmental context. Mercury, in its methylated form, is a neurotoxin that biomagnifies in marine and terrestrial foodwebs leading to elevated levels in fish and fish-eating mammals worldwide, including at numerous Arctic locations. Elevated mercury concentrations in Arctic country foods present a significant exposure risk to Arctic people. We present a detailed review of the fate of mercury in Arctic terrestrial and marine ecosystems, taking into account the extreme seasonality of Arctic ecosystems and the unique processes associated with sea ice and Arctic hydrology.

Are Arctic Ocean ecosystems exceptionally vulnerable to global emissions of mercury? A call for emphasised research on methylation and the consequences of climate change

Environmental Chemistry, 2010

Environmental context. Mercury is a global contaminant that has entered Arctic food webs in sufficient quantity to put at risk the health of top predators and humans that consume them. Recent research has discovered a photochemical process unique to the Arctic that leads to mercury deposition on frozen surfaces after polar sunrise, but the connection between mercury deposition and entry into food webs remains tenuous and poorly understood. We propose here that the Arctic Ocean's sensitivity to the global mercury cycle depends far more on neglected post-deposition processes that lead to methylation within the ice-ocean system, and the vulnerability of these processes to changes occurring in the cryosphere.

Arctic Ocean: Is It a Sink or a Source of Atmospheric Mercury?

Environmental Science & Technology, 2014

High levels of mercury in marine mammals threaten the health of Arctic inhabitants. Whether the Arctic Ocean (AO) is a sink or a source of atmospheric mercury is unknown. Given the paucity of observations in the Arctic, models are useful in addressing this question. GEOS-Chem and GRAHM, two complex numerical mercury models, present contrasting pictures of atmospheric mercury input to AO at 45 and 108 Mg yr −1 , respectively, and ocean evasion at 90 and 33 Mg yr −1 , respectively. We provide a comprehensive evaluation of GRAHM simulated atmospheric mercury input to AO using mercury observations in air, precipitation and snowpacks, and an analysis of the discrepancy between the two modeling estimates using observations. We discover two peaks in high-latitude summertime concentrations of atmospheric mercury. We show that the first is caused mainly by snowmelt revolatilization and the second by AO evasion of mercury. Riverine mercury export to AO is estimated at 50 Mg yr −1 based on measured DOC export and at 15.5−31 Mg yr −1 based on simulated mercury in meltwater. The range of simulated mercury fluxes to and from AO reflects uncertainties in modeling mercury in the Arctic; comprehensive observations in all compartments of the Arctic ecosystem are needed to close the gap.

Temporal trends of Hg in Arctic biota, an update

Science of The Total Environment, 2011

A statistically robust method was applied to 83 time-series of mercury in Arctic biota from marine, freshwater and terrestrial ecosystems with the purpose of generating a ‘meta-analysis’ of temporal trend data collected over the past two to three decades, mostly under the auspices of the Arctic Monitoring and Assessment Program (AMAP). Sampling locations ranged from Alaska in the west to

Subsurface seawater methylmercury maximum explains biotic mercury concentrations in the Canadian Arctic

Scientific Reports, 2018

Mercury (Hg) is a contaminant of major concern in Arctic marine ecosystems. Decades of Hg observations in marine biota from across the Canadian Arctic show generally higher concentrations in the west than in the east. Various hypotheses have attributed this longitudinal biotic Hg gradient to regional differences in atmospheric or terrestrial inputs of inorganic Hg, but it is methylmercury (MeHg) that accumulates and biomagnifies in marine biota. Here, we present high-resolution vertical profiles of total Hg and MeHg in seawater along a transect from the Canada Basin, across the Canadian Arctic Archipelago (CAA) and Baffin Bay, and into the Labrador Sea. Total Hg concentrations are lower in the western Arctic, opposing the biotic Hg distributions. In contrast, MeHg exhibits a distinctive subsurface maximum at shallow depths of 100-300 m, with its peak concentration decreasing eastwards. As this subsurface MeHg maximum lies within the habitat of zooplankton and other lower trophic-level biota, biological uptake of subsurface MeHg and subsequent biomagnification readily explains the biotic Hg concentration gradient. Understanding the risk of MeHg to the Arctic marine ecosystem and Indigenous Peoples will thus require an elucidation of the processes that generate and maintain this subsurface MeHg maximum. Monitoring data collected during the past four decades have shown Hg concentrations in Canadian Arctic marine mammals (e.g., beluga whales, ringed seals, polar bears) to be highly elevated, frequently exceeding toxicity thresholds 1,2. This has raised major concerns over the health of marine mammals and Indigenous Peoples whose traditional diets include marine mammal tissues. Mercury concentrations in marine biota are generally higher in the Beaufort Sea and western Canadian Arctic Archipelago (CAA) than in the eastern CAA and Baffin Bay 1-3. This longitudinal gradient is not limited to apex predators 4,5 , but extends to organisms at lower trophic levels such as zooplankton (e.g., Themisto spp., Calanus spp.) 6 (Fig. 1a). Whereas regional variations in top predator Hg concentrations may be linked to feeding behavior and dietary preference 5 , observed spatial patterns persist after adjustments are made to account for trophic position 3. Extensive efforts have been made to identify factors that control the spatial trends in marine biota and to develop appropriate mitigation strategies to reduce biotic Hg concentrations. Most hypotheses attribute higher marine biotic Hg concentrations in the western Canadian Arctic to elevated inputs of inorganic Hg to these regions. These inputs include (1) atmospheric deposition of anthropogenic Hg from Asian sources 3 , which is enhanced locally by atmospheric mercury depletion events (AMDEs) during polar sunrise 7 ; (2) riverine Hg input from the Mackenzie River 8,9 , which may be enhanced by tundra uptake of atmospheric elemental Hg 10 [and permafrost thawing 11 ; and (3) a naturally high geological background of Hg 12. These inorganic Hg-based hypotheses do not account for the fact that it is methylmercury (MeHg), not inorganic Hg, that accumulates and biomagnifies in marine biota 2. The discovery of a subsurface MeHg enrichment in global oceans 13-16 suggests that seawater MeHg may play a more important role in determining marine biotic Hg concentrations 17,18 , especially in regions such as the Beaufort Sea 15 and the central Arctic Ocean 16 where the maximum MeHg concentration was observed at shallow depths.

What is the fate of mercury entering the Arctic environment?

Environmental context. Mercury, in its methylated form, is a neurotoxin that biomagnifies in marine and terrestrial foodwebs leading to elevated levels in fish and fish-eating mammals worldwide, including at numerous Arctic locations. Elevated mercury concentrations in Arctic country foods present a significant exposure risk to Arctic people. We present a detailed review of the fate of mercury in Arctic terrestrial and marine ecosystems, taking into account the extreme seasonality of Arctic ecosystems and the unique processes associated with sea ice and Arctic hydrology.

The Arctic: a sink for mercury

Tellus B, 2004

A B S T R A C T Mercury is a persistent, toxic and bio-accumulative pollutant of global interest. Its main mass in the troposphere is in the form of elemental gas-phase mercury. Rapid, near-complete depletion of mercury has been observed during spring in the atmospheric boundary layer of frozen marine areas in Arctic, sub-Arctic and Antarctic locations. It is strongly correlated with ozone depletion. To date, evidence has indicated strongly that chemistry involving halogen gases from surface sea-salt is the mechanism of this destruction. Precisely which halogen gases are the main players has remained unresolved. Our novel kinetic data and multiscale modelling show that Br atoms and BrO radicals are the most effective halogens driving mercury oxidation. The reduction of oxidized mercury deposited in the snow pack back to Hg 0 and subsequent diffusion to the atmosphere is observed. However, it cannot compensate for the total deposition, and a net accumulation occurs. We use a unique global atmospheric mercury model to estimate that halogen-driven mercury depletion events result in a 44% increase in the net deposition of mercury to the Arctic. Over a 1-yr cycle, we estimate an accumulation of 325 tons of mercury in the Arctic.