scholarly journals Mercury cycling in the Arctic - does enhanced deposition flux mean net-input?

2008 ◽  
Vol 5 (2) ◽  
pp. 87 ◽  
Author(s):  
Ralf Ebinghaus

Environmental context. Mercury has unique physico-chemical characteristics that include long-range atmospheric transport, transformation into highly toxic methylmercury species, and the bioaccumulation of these compounds, especially in the marine environment. This has motivated intense international research on mercury as a pollutant of global concern. With respect to Polar regions, scientific interest and research activities were even accelerated after the discovery of the so-called atmospheric mercury depletion events (AMDEs), which are supposed to lead to enhanced mercury deposition flux into these pristine environments in the ecologically very sensitive period in polar spring.

2010 ◽  
Vol 10 (24) ◽  
pp. 12037-12057 ◽  
Author(s):  
C. D. Holmes ◽  
D. J. Jacob ◽  
E. S. Corbitt ◽  
J. Mao ◽  
X. Yang ◽  
...  

Abstract. Global models of atmospheric mercury generally assume that gas-phase OH and ozone are the main oxidants converting Hg0 to HgII and thus driving mercury deposition to ecosystems. However, thermodynamic considerations argue against the importance of these reactions. We demonstrate here the viability of atomic bromine (Br) as an alternative Hg0 oxidant. We conduct a global 3-D simulation with the GEOS-Chem model assuming gas-phase Br to be the sole Hg0 oxidant (Hg + Br model) and compare to the previous version of the model with OH and ozone as the sole oxidants (Hg + OH/O3 model). We specify global 3-D Br concentration fields based on our best understanding of tropospheric and stratospheric Br chemistry. In both the Hg + Br and Hg + OH/O3 models, we add an aqueous photochemical reduction of HgII in cloud to impose a tropospheric lifetime for mercury of 6.5 months against deposition, as needed to reconcile observed total gaseous mercury (TGM) concentrations with current estimates of anthropogenic emissions. This added reduction would not be necessary in the Hg + Br model if we adjusted the Br oxidation kinetics downward within their range of uncertainty. We find that the Hg + Br and Hg + OH/O3 models are equally capable of reproducing the spatial distribution of TGM and its seasonal cycle at northern mid-latitudes. The Hg + Br model shows a steeper decline of TGM concentrations from the tropics to southern mid-latitudes. Only the Hg + Br model can reproduce the springtime depletion and summer rebound of TGM observed at polar sites; the snowpack component of GEOS-Chem suggests that 40% of HgII deposited to snow in the Arctic is transferred to the ocean and land reservoirs, amounting to a net deposition flux to the Arctic of 60 Mg a−1. Summertime events of depleted Hg0 at Antarctic sites due to subsidence are much better simulated by the Hg + Br model. Model comparisons to observed wet deposition fluxes of mercury in the US and Europe show general consistency. However the Hg + Br model does not capture the summer maximum over the southeast US because of low subtropical Br concentrations while the Hg + OH/O3 model does. Vertical profiles measured from aircraft show a decline of Hg0 above the tropopause that can be captured by both the Hg + Br and Hg + OH/O3 models, except in Arctic spring where the observed decline is much steeper than simulated by either model; we speculate that oxidation by Cl species might be responsible. The Hg + Br and Hg + OH/O3 models yield similar global budgets for the cycling of mercury between the atmosphere and surface reservoirs, but the Hg + Br model results in a much larger fraction of mercury deposited to the Southern Hemisphere oceans.


Atmosphere ◽  
2021 ◽  
Vol 13 (1) ◽  
pp. 37
Author(s):  
Stella Eyrikh ◽  
Liliya Shol ◽  
Elena Shinkaruk

The problem of mercury input and its further distribution in the Arctic environment is actively debated, especially in recent times, due to the observed processes of permafrost thawing causing the enhanced release of mercury into the Arctic atmosphere and further distribution in the terrestrial and aquatic ecosystem. The atmospheric mercury deposition occurs via dry deposition and wet scavenging by precipitation events. Here we present a study of Hg in wet precipitation on the remote territory of the Russian Arctic; the data were obtained at the monitoring stations Nadym and Salekhard in 2016–2018. Mercury pollution of the Salekhard atmosphere in cold time is mainly determined by regional and local sources, while in Nadym, long-range transport of mercury and local fuel combustion are the main sources of pollutants in the cold season, while internal regional sources have a greater impact on the warm season. Total mercury concentrations in wet precipitation in Nadym varied from <0.5 to 63.3 ng/L. The highest Hg concentrations in the springtime were most likely attributed to atmospheric mercury depletion events (AMDE). The contributions of wet atmospheric precipitation during the AMDE period to the annual Hg deposition were 16.7% and 9.8% in 2016/2017 and 2017/2018, respectively. The average annual volume-weighted Hg concentration (VWC) in the atmospheric precipitation in Nadym is notably higher than the values reported for the remote regions in the Arctic and comparable with the values obtained for the other urbanized regions of the world. Annual Hg fluxes in Nadym are nevertheless close to the average annual fluxes for remote territories of the Arctic zone and significantly lower than the annual fluxes reported for unpolluted sites of continental-scale monitoring networks of the different parts of the world (USA, Europe, and China). The increase of Hg deposition flux with wet precipitation in Nadym in 2018 might be caused by regional emissions of gas and oil combustion, wildfires, and Hg re-emission from soils due to the rising air temperature. The 37 cm increase of the seasonally thawed layer (STL) in 2018 compared to the 10-year average reflects that the climatic changes in the Nadym region might increase Hg(0) evasion, considering a great pool of Hg is contained in permafrost.


2010 ◽  
Vol 10 (8) ◽  
pp. 19845-19900 ◽  
Author(s):  
C. D. Holmes ◽  
D. J. Jacob ◽  
E. S. Corbitt ◽  
J. Mao ◽  
X. Yang ◽  
...  

Abstract. Global models of atmospheric mercury generally assume that OH and ozone are the main oxidants converting Hg0 to HgII and thus driving mercury deposition to ecosystems. However, thermodynamic considerations argue against the importance of these reactions. We demonstrate here the viability of atomic bromine (Br) as an alternative Hg0 oxidant. We conduct a global 3-D simulation with the GEOS-Chem model assuming Br to be the sole Hg0 oxidant (Hg + Br model) and compare to the previous version of the model with OH and ozone as the sole oxidants (Hg + OH/O3 model). We specify global 3-D Br concentration fields based on our best understanding of tropospheric and stratospheric Br chemistry. In both the Hg + Br and Hg + OH/O3 models, we add an aqueous photochemical reduction of HgII in cloud to impose a tropospheric lifetime for mercury of 6.5 months against deposition, as needed to reconcile observed total gaseous mercury (TGM) concentrations with current estimates of anthropogenic emissions. This added reduction would not be necessary in the Hg + Br model if we adjusted the Br oxidation kinetics downward within their range of uncertainty. We find that the Hg + Br and Hg + OH/O3 models are equally capable of reproducing the spatial distribution of TGM and its seasonal cycle at northern mid-latitudes. The Hg + Br model shows a steeper decline of TGM concentrations from the tropics to southern mid-latitudes. Only the Hg + Br model can reproduce the springtime depletion and summer rebound of TGM observed at polar sites; the snowpack component of GEOS-Chem suggests that 40% of HgII deposited to snow in the Arctic is transferred to the ocean and land reservoirs, amounting to a net deposition flux of 60 Mg a−1. Summertime events of depleted Hg0 at Antarctic sites due to subsidence are much better simulated by the Hg + Br model. Model comparisons to observed wet deposition fluxes of mercury in the US and Europe show general consistency but the Hg + Br model is unable to capture the summer maximum over the southeast US because of low subtropical Br concentrations. Vertical profiles measured from aircraft show a decline of Hg0 above the tropopause that can be captured by both the Hg + Br and Hg + OH/O3 models, except in Arctic spring where the observed decline is much steeper than simulated by either model; we speculate that oxidation by Cl species might be responsible. The Hg + Br and Hg + OH/O3 models yield similar global budgets for the cycling of mercury between the atmosphere and surface reservoirs, but the Hg + Br model results in much larger fraction of mercury deposited to the Southern Hemisphere oceans.


2014 ◽  
Vol 14 (5) ◽  
pp. 2233-2244 ◽  
Author(s):  
J. Zhu ◽  
T. Wang ◽  
R. Talbot ◽  
H. Mao ◽  
X. Yang ◽  
...  

Abstract. A comprehensive measurement study of mercury wet deposition and size-fractionated particulate mercury (HgP) concurrent with meteorological variables was conducted from June 2011 to February 2012 to evaluate the characteristics of mercury deposition and particulate mercury in urban Nanjing, China. The volume-weighted mean (VWM) concentration of mercury in rainwater was 52.9 ng L−1 with a range of 46.3–63.6 ng L−1. The wet deposition per unit area was averaged 56.5 μg m−2 over 9 months, which was lower than that in most Chinese cities, but much higher than annual deposition in urban North America and Japan. The wet deposition flux exhibited obvious seasonal variation strongly linked with the amount of precipitation. Wet deposition in summer contributed more than 80% to the total amount. A part of contribution to wet deposition of mercury from anthropogenic sources was evidenced by the association between wet deposition and sulfates, as well as nitrates in rainwater. The ions correlated most significantly with mercury were formate, calcium, and potassium, which suggested that natural sources including vegetation and resuspended soil should be considered as an important factor to affect the wet deposition of mercury in Nanjing. The average HgP concentration was 1.10 ± 0.57 ng m−3. A distinct seasonal distribution of HgP concentrations was found to be higher in winter as a result of an increase in the PM10 concentration. Overall, more than half of the HgP existed in the particle size range less than 2.1 μm. The highest concentration of HgP in coarse particles was observed in summer, while HgP in fine particles dominated in fall and winter. The size distribution of averaged mercury content in particulates was bimodal, with two peaks in the bins of < 0.7 μm and 4.7–5.8 μm. Dry deposition per unit area of HgP was estimated to be 47.2 μg m−2 using meteorological conditions and a size-resolved particle dry deposition model. This was 16.5% less than mercury wet deposition. Compared to HgP in fine particles, HgP in coarse particles contributed more to the total dry deposition due to higher deposition velocities. Negative correlation between precipitation and the HgP concentration reflected the effect of scavenging of HgP by precipitation.


2007 ◽  
Vol 7 (4) ◽  
pp. 10837-10931 ◽  
Author(s):  
A. Steffen ◽  
T. Douglas ◽  
M. Amyot ◽  
P. Ariya ◽  
K. Aspmo ◽  
...  

Abstract. It was discovered in 1995 that, during the spring time, unexpectedly low concentrations of gaseous elemental mercury (GEM) occurred in the Arctic air. This was surprising for a pollutant known to have a long residence time in the atmosphere; however conditions appeared to exist in the Arctic that promoted this depletion of mercury (Hg). This phenomenon is termed atmospheric mercury depletion events (AMDEs) and its discovery has revolutionized our understanding of the cycling of Hg in Polar Regions while stimulating a significant amount of research to understand its impact to this fragile ecosystem. Shortly after the discovery was made in Canada, AMDEs were confirmed to occur throughout the Arctic, sub-Artic and Antarctic coasts. It is now known that, through a series of photochemically initiated reactions involving halogens, GEM is converted to a more reactive species and is subsequently associated to particles in the air and/or deposited to the polar environment. AMDEs are a means by which Hg is transferred from the atmosphere to the environment that was previously unknown. In this article we review the history of Hg in Polar Regions, the methods used to collect Hg in different environmental media, research results of the current understanding of AMDEs from field, laboratory and modeling work, how Hg cycles around the environment after AMDEs, gaps in our current knowledge and the future impacts that AMDEs may have on polar environments. The research presented has shown that while considerable improvements in methodology to measure Hg have been made the main limitation remains knowing the speciation of Hg in the various media. The processes that drive AMDEs and how they occur are discussed. As well, the roles that the snow pack, oceans, fresh water and the sea ice play in the cycling of Hg are presented. It has been found that deposition of Hg from AMDEs occurs at marine coasts and not far inland and that a fraction of the deposited Hg does not remain in the same form in the snow. Kinetic studies undertaken have demonstrated that bromine is the major oxidant depleting Hg in the atmosphere. Modeling results demonstrate that there is a significant deposition of Hg to Polar Regions as a result of AMDEs. Models have also shown that Hg is readily transported to the Arctic from source regions, at times during springtime when this environment is actively transforming Hg from the atmosphere to the snow and ice surfaces. The presence of significant amounts of methyl Hg in snow in the Arctic surrounding AMDEs is important because this species is the link between the environment and impacts to wildlife and humans. Further, much work on methylation and demethylation processes have occurred but are not yet fully understood. Recent changes in the climate and sea ice cover in Polar Regions are likely to have strong effects on the cycling of Hg in this environment; however more research is needed to understand Hg processes in order to formulate meaningful predictions of these changes. Mercury, Atmospheric mercury depletion events (AMDE), Polar, Arctic, Antarctic, Ice


2018 ◽  
Vol 18 (24) ◽  
pp. 17895-17907 ◽  
Author(s):  
Oscar B. Dimdore-Miles ◽  
Paul I. Palmer ◽  
Lori P. Bruhwiler

Abstract. We consider the utility of the annual inter-polar difference (IPD) as a metric for changes in Arctic emissions of methane (CH4). The IPD has been previously defined as the difference between weighted annual means of CH4 mole fraction data collected at stations from the two polar regions (defined as latitudes poleward of 53∘ N and 53∘ S, respectively). This subtraction approach (IPD) implicitly assumes that extra-polar CH4 emissions arrive within the same calendar year at both poles. We show using a continuous version of the IPD that the metric includes not only changes in Arctic emissions but also terms that represent atmospheric transport of air masses from lower latitudes to the polar regions. We show the importance of these atmospheric transport terms in understanding the IPD using idealized numerical experiments with the TM5 global 3-D atmospheric chemistry transport model that is run from 1980 to 2010. A northern mid-latitude pulse in January 1990, which increases prior emission distributions, arrives at the Arctic with a higher mole fraction and ≃12 months earlier than at the Antarctic. The perturbation at the poles subsequently decays with an e-folding lifetime of ≃4 years. A similarly timed pulse emitted from the tropics arrives with a higher value at the Antarctic ≃11 months earlier than at the Arctic. This perturbation decays with an e-folding lifetime of ≃7 years. These simulations demonstrate that the assumption of symmetric transport of extra-polar emissions to the poles is not realistic, resulting in considerable IPD variations due to variations in emissions and atmospheric transport. We assess how well the annual IPD can detect a constant annual growth rate of Arctic emissions for three scenarios, 0.5 %, 1 %, and 2 %, superimposed on signals from lower latitudes, including random noise. We find that it can take up to 16 years to detect the smallest prescribed trend in Arctic emissions at the 95 % confidence level. Scenarios with higher, but likely unrealistic, growth in Arctic emissions are detected in less than a decade. We argue that a more reliable measurement-driven approach would require data collected from all latitudes, emphasizing the importance of maintaining a global monitoring network to observe decadal changes in atmospheric greenhouse gases.


2008 ◽  
Vol 8 (6) ◽  
pp. 1445-1482 ◽  
Author(s):  
A. Steffen ◽  
T. Douglas ◽  
M. Amyot ◽  
P. Ariya ◽  
K. Aspmo ◽  
...  

Abstract. It was discovered in 1995 that, during the spring time, unexpectedly low concentrations of gaseous elemental mercury (GEM) occurred in the Arctic air. This was surprising for a pollutant known to have a long residence time in the atmosphere; however conditions appeared to exist in the Arctic that promoted this depletion of mercury (Hg). This phenomenon is termed atmospheric mercury depletion events (AMDEs) and its discovery has revolutionized our understanding of the cycling of Hg in Polar Regions while stimulating a significant amount of research to understand its impact to this fragile ecosystem. Shortly after the discovery was made in Canada, AMDEs were confirmed to occur throughout the Arctic, sub-Artic and Antarctic coasts. It is now known that, through a series of photochemically initiated reactions involving halogens, GEM is converted to a more reactive species and is subsequently associated to particles in the air and/or deposited to the polar environment. AMDEs are a means by which Hg is transferred from the atmosphere to the environment that was previously unknown. In this article we review Hg research taken place in Polar Regions pertaining to AMDEs, the methods used to collect Hg in different environmental media, research results of the current understanding of AMDEs from field, laboratory and modeling work, how Hg cycles around the environment after AMDEs, gaps in our current knowledge and the future impacts that AMDEs may have on polar environments. The research presented has shown that while considerable improvements in methodology to measure Hg have been made but the main limitation remains knowing the speciation of Hg in the various media. The processes that drive AMDEs and how they occur are discussed. As well, the role that the snow pack and the sea ice play in the cycling of Hg is presented. It has been found that deposition of Hg from AMDEs occurs at marine coasts and not far inland and that a fraction of the deposited Hg does not remain in the same form in the snow. Kinetic studies undertaken have demonstrated that bromine is the major oxidant depleting Hg in the atmosphere. Modeling results demonstrate that there is a significant deposition of Hg to Polar Regions as a result of AMDEs. Models have also shown that Hg is readily transported to the Arctic from source regions, at times during springtime when this environment is actively transforming Hg from the atmosphere to the snow and ice surfaces. The presence of significant amounts of methyl Hg in snow in the Arctic surrounding AMDEs is important because this species is the link between the environment and impacts to wildlife and humans. Further, much work on methylation and demethylation processes has occurred but these processes are not yet fully understood. Recent changes in the climate and sea ice cover in Polar Regions are likely to have strong effects on the cycling of Hg in this environment; however more research is needed to understand Hg processes in order to formulate meaningful predictions of these changes.


2010 ◽  
Vol 10 (5) ◽  
pp. 11577-11614 ◽  
Author(s):  
I. Stemmler ◽  
G. Lammel

Abstract. Perfluorooctanoic acid (PFOA) and other perfluorinated compounds are industrial chemicals in use since decades which resist degradation in the environment and seem to accumulate in polar regions. Transport of PFOA was modeled using a spatially resolved global multicompartment model including fully coupled three-dimensional ocean and atmosphere general circulation models, and two-dimensional top soil, vegetation surfaces, and sea ice compartments. In addition to primary emissions, the formation of PFOA in the atmosphere from degradation of 8:2 fluorotelomer alcohol was included as a PFOA source. Oceanic transport, delivered 14.8±5.0 (8–23) t a−1 to the Arctic, strongly influenced by changes in water transport, which determined its interannual variability. This pathway constituted the dominant source of PFOA to the Arctic. Formation of PFOA in the atmosphere lead to episodic transport events (timescale of days) into the Arctic with small spatial extent. Deposition in the polar region was found to be dominated by wet deposition over land, and shows maxima in boreal winter. The total atmospheric deposition of PFOA in the Arctic in the 1990s was ≈1 t a−1, much higher than previously estimated, and is dominated by primary emissions rather than secondarily formed.


Geosciences ◽  
2018 ◽  
Vol 8 (10) ◽  
pp. 374 ◽  
Author(s):  
Marta Pérez-Rodríguez ◽  
Olga Margalef ◽  
Juan Corella ◽  
Alfonso Saiz-Lopez ◽  
Sergi Pla-Rabes ◽  
...  

The study of mercury accumulation in peat cores provides an excellent opportunity to improve the knowledge on mercury cycling and depositional processes at remote locations far from pollution sources. We analyzed mercury concentrations in 150 peat samples from two cores from Rano Aroi (Easter Island, 27° S) and in selected vegetation samples of present-day flora of the island, in order to characterize the mercury cycling for the last ~71 ka BP. The mercury concentrations showed values ranging between 35 and 200 ng g−1, except for a large maxima (~1000 ng g−1) which occurred at the end of the Last Glacial Maximum (LGM, ~20 ka cal BP) in both peat cores. Low temperatures during the LGM would accelerate the atmospheric oxidation of Hg(0) to divalent mercury that, coupled with higher rainfall during this period, most likely resulted in a very efficient surface deposition of atmospheric mercury. Two exceptional short-lived Hg peaks occurred during the Holocene at 8.5 (350 ng g−1) and 4.7 (1000 ng g−1) ka cal BP. These values are higher than those recorded in most peat records belonging to the industrial period, highlighting that natural factors played a significant role in Hg accumulation—sometimes even more so than anthropogenic sources. Our results suggest that wet deposition, linked to atmospheric oxidation, was the main process controlling the short-lived Hg events, both in the mire and in the catchment soils.


2001 ◽  
Vol 28 (17) ◽  
pp. 3219-3222 ◽  
Author(s):  
Julia Y. Lu ◽  
William H. Schroeder ◽  
Len A. Barrie ◽  
Alexandra Steffen ◽  
Harold E. Welch ◽  
...  

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