scholarly journals Depletion of atmospheric gaseous elemental mercury by plant uptake at Mt. Changbai, Northeast China

Author(s):  
Xuewu Fu ◽  
Wei Zhu ◽  
Hui Zhang ◽  
Jonas Sommar ◽  
Xu Yang ◽  
...  

Abstract. There exists observational evidence that GEM can be readily removed from the atmosphere via chemical oxidation followed by deposition in the polar and sub-polar regions, free troposphere, lower stratosphere, and marine boundary layer under specific environmental conditions. Here we report GEM depletions in a temperate mixed forest at Mt. Changbai, Northeast China. The depletion occurred exclusively at night during leaf-growing season and in the absence of GOM enrichment (GOM 

2016 ◽  
Vol 16 (20) ◽  
pp. 12861-12873 ◽  
Author(s):  
Xuewu Fu ◽  
Wei Zhu ◽  
Hui Zhang ◽  
Jonas Sommar ◽  
Ben Yu ◽  
...  

Abstract. There exists observational evidence that gaseous elemental mercury (GEM) can be readily removed from the atmosphere via chemical oxidation followed by deposition in the polar and sub-polar regions, free troposphere, lower stratosphere, and marine boundary layer under specific environmental conditions. Here we report GEM depletions in a temperate mixed forest at Mt. Changbai, Northeast China. The strong depletions occurred predominantly at night during the leaf-growing season and in the absence of gaseous oxidized mercury (GOM) enrichment (GOM  <  3 pg m−3). Vertical gradients of decreasing GEM concentrations from layers above to under forest canopy suggest in situ loss of GEM to forest canopy at Mt. Changbai. Foliar GEM flux measurements showed that the foliage of two predominant tree species is a net sink of GEM at night, with a mean flux of −1.8 ± 0.3 ng m2 h−1 over Fraxinus mandshurica (deciduous tree species) and −0.1 ± 0.2 ng m2 h−1 over Pinus Koraiensis (evergreen tree species). Daily integrated GEM δ202Hg, Δ199Hg, and Δ200Hg at Mt. Changbai during 8–18 July 2013 ranged from −0.34 to 0.91 ‰, from −0.11 to −0.04 ‰ and from −0.06 to 0.01 ‰, respectively. A large positive shift in GEM δ202Hg occurred during the strong GEM depletion events, whereas Δ199Hg and Δ200Hg remained essentially unchanged. The observational findings and box model results show that uptake of GEM by forest canopy plays a predominant role in the GEM depletion at Mt. Changbai forest. Such depletion events of GEM are likely to be a widespread phenomenon, suggesting that the forest ecosystem represents one of the largest sinks ( ∼ 1930 Mg) of atmospheric Hg on a global scale.


2010 ◽  
Vol 10 (3) ◽  
pp. 1121-1131 ◽  
Author(s):  
E.-G. Brunke ◽  
C. Labuschagne ◽  
R. Ebinghaus ◽  
H. H. Kock ◽  
F. Slemr

Abstract. Gaseous mercury in the marine boundary layer has been measured with a 15 min temporal resolution at the Global Atmosphere Watch station Cape Point since March 2007. The most prominent features of the data until July 2008 are the frequent occurrences of pollution (PEs) and depletion events (DEs). Both types of events originate mostly within a short transport distance (up to about 100 km), which are embedded in air masses ranging from marine background to continental. The Hg/CO emission ratios observed during the PEs are within the range reported for biomass burning and industrial/urban emissions. The depletion of gaseous mercury during the DEs is in many cases almost complete and suggests an atmospheric residence time of elemental mercury as short as a few dozens of hours, which is in contrast to the commonly used estimate of approximately 1 year. The DEs observed at Cape Point are not accompanied by simultaneous depletion of ozone which distinguishes them from the halogen driven atmospheric mercury depletion events (AMDEs) observed in Polar Regions. Nonetheless, DEs similar to those observed at Cape Point have also been observed at other places in the marine boundary layer. Additional measurements of mercury speciation and of possible mercury oxidants are hence called for to reveal the chemical mechanism of the newly observed DEs and to assess its importance on larger scales.


2010 ◽  
Vol 7 (6) ◽  
pp. 537 ◽  
Author(s):  
Anne L. Soerensen ◽  
Henrik Skov ◽  
Matthew S. Johnson ◽  
Marianne Glasius

Environmental context Mercury is a neurotoxin that bioaccumulates in the aquatic food web. Atmospheric emissions from urban areas close to the coast could cause increased local mercury deposition to the ocean. Our study adds important new data to the current limited knowledge on atmospheric mercury emissions and dynamics in coastal urban areas. Abstract Approximately 50% of primary atmospheric mercury emissions are anthropogenic, resulting from e.g. emission hotspots in urban areas. Emissions from urban areas close to the coast are of interest because they could increase deposition loads to nearby coastal waters as well as contribute to long range transport of mercury. We present results from measurements of gaseous elemental mercury (GEM) and reactive gaseous mercury (RGM) in 15 coastal cities and their surrounding marine boundary layer (MBL). An increase of 15–90% in GEM concentration in coastal urban areas was observed compared with the remote MBL. Strong RGM enhancements were only found in two cities. In urban areas with statistically significant GEM/CO enhancement ratios, slopes between 0.0020 and 0.0087 ng m–3 ppb–1 were observed, which is consistent with other observations of anthropogenic enhancement. The emission ratios were used to estimate GEM emissions from the areas. A closer examination of data from Sydney (Australia), the coast of Chile, and Valparaiso region (Chile) in the southern hemisphere, is presented.


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


2017 ◽  
Author(s):  
Maor Gabay ◽  
Mordechai Peleg ◽  
Erick Fredj ◽  
Eran Tas

Abstract. Accurate characterization of gaseous elemental mercury (GEM) chemical oxidation pathways and their kinetics is critically important for assessing the transfer of atmospheric mercury to bioaquatic systems. Recent comprehensive field measurements have suggested that the nitrate radical (NO3) plays a role in efficient nighttime oxidation of GEM, and that the role of the hydroxyl radical (OH) as a GEM oxidant has been underestimated. We used the CAABA/MECCA chemical box model and additional kinetic calculations to analyze these measurement results, in order to investigate the nighttime and daytime oxidation of GEM. We assumed a second-order reaction for the NO3 induced nighttime oxidation of GEM. Our analysis demonstrated that nighttime oxidation of GEM has to be included in the model to account for the measured variations in nighttime reactive gaseous mercury (RGM) concentration. A lower limit and best-fit rate constant for GEM nighttime oxidation are provided. To the best of our knowledge, this is the first time that a rate for nighttime oxidation of GEM has been determined based on field measurements. Our analysis further indicates that OH has a much more important role in GEM oxidation than commonly considered. A lower-limit rate constant for the OH–RGM reaction is provided.


2016 ◽  
Author(s):  
Z. Ye ◽  
H. Mao ◽  
C.-J. Lin ◽  
S. Y. Kim

Abstract. A box model incorporating a state-of-the-art chemical mechanism for atmospheric mercury (Hg) cycling was developed to investigate oxidation of gaseous elemental mercury (GEM) at three locations in the northeastern United States: Appledore Island (marine), Thompson Farm (coastal, rural), and Pack Monadnock (inland, rural, elevated). The chemical mechanism improved model's ability to simulate the formation of gaseous oxidized mercury (GOM) at the study sites. At the coastal and inland sites, GEM oxidation was predominated by O3 and OH, contributing 80–99 % of total GOM production during daytime. H2O2 initiated GEM oxidation was significant (~ 33 % of the total GOM) at the inland site during nighttime. In the marine boundary layer (MBL), Br and BrO were dominant GEM oxidants contributing ~ 70 % of the total GOM production during mid-day, while O3 dominated GEM oxidation (50–90 % of GOM production) over the remaining day. Following the production of HgBr from GEM + Br, HgBr was oxidized by BrO, HO2, OH, ClO, and IO to form Hg(II) brominated GOM species. However, under atmospheric conditions, the prevalent GEM oxidants in the MBL could be Br / BrO or O3 / OH depending on Br and BrO mixing ratios. Relative humidity and products of the CH3O2 + BrO reaction possibly affected significantly the mixing ratios of Br or BrO radicals and subsequently GOM formation. Gas-particle partitioning could be potentially important in the production of GOM as well as Br and BrO at the marine site.


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.


2012 ◽  
Vol 12 (11) ◽  
pp. 5099-5112 ◽  
Author(s):  
H. Mao ◽  
R. Talbot

Abstract. A comprehensive analysis was conducted using long-term continuous measurements of gaseous elemental mercury (Hg0), reactive gaseous mercury (RGM), and particulate phase mercury (HgP) at coastal (Thompson Farm, denoted as TF), marine (Appledore Island, denoted as AI), and elevated inland (Pac Monadnock, denoted as PM) sites from the AIRMAP Observatories in southern New Hampshire, USA. Decreasing trends in background Hg0 were identified in the 7.5- and 5.5-yr records at TF and PM with decline rates of 3.3 parts per quadrillion by volume (ppqv) yr−1 and 6.3 ppqv yr−1, respectively. Common characteristics at these sites were the reproducible annual cycle of Hg0 with its maximum in winter-spring and minimum in fall, comprised of a positive trend in the warm season (spring – early fall) and a negative one in the cool season (late fall – winter). Year-to-year variability was observed in the warm season decline in Hg0 at TF varying from a minimum total (complete) seasonal loss of 43 ppqv in 2009 to a maximum of 92 ppqv in 2005, whereas variability remained small at AI and PM. The coastal site TF differed from the other two sites with its exceptionally low levels (as low as below 50 ppqv) in the nocturnal inversion layer possibly due to dissolution in dew water. Measurements of Hg0 at PM exhibited the smallest diurnal to annual variability among the three environments, where peak levels rarely exceeded 250 ppqv and the minimum was typically 100 ppqv. It should be noted that summertime diurnal patterns at TF and AI were opposite in phase indicating strong sink(s) for Hg0 during the day in the marine boundary layer, which was consistent with the hypothesis of Hg0 oxidation by halogen radicals there. Mixing ratios of RGM in the coastal and marine boundary layers reached annual maxima in spring and minima in fall, whereas at PM levels were generally below the limit of detection (LOD) except in spring. RGM levels at AI were higher than at TF and PM indicating a stronger source strength in the marine environment. Mixing ratios of HgP at AI and TF were close in magnitude to RGM levels and were mostly below 1 ppqv. Diurnal variation in HgP was barely discernible at TF and AI in spring and summer. Higher levels of HgP were observed during the day, while values that were smaller, but above the LOD, occurred at night.


2020 ◽  
Author(s):  
Lena Wohlgemuth ◽  
Stefan Osterwalder ◽  
Günter Hoch ◽  
Christine Alewell ◽  
Martin Jiskra

&lt;p&gt;The deposition of gaseous elemental mercury, Hg(0), from the atmosphere to terrestrial surfaces remains poorly understood mainly due to difficulties in measuring net Hg(0) fluxes on the ecosystem scale. However, there is emerging evidence that vegetation uptake of atmospheric Hg(0) represents a major deposition pathway to terrestrial surfaces. We will present a novel bottom up approach to calculate Hg(0) deposition fluxes to aboveground foliage by combining foliar Hg accumulation rates on the basis of leaf area with species-specific leaf area indices. We analyzed Hg content in 583 foliage samples from major tree species at 10 European forested research sites along a latitudinal gradient from Switzerland to Northern Finland over the course of the 2018 growing season. Foliar Hg concentrations increased over time in all tree species at all sites. We found that foliar Hg accumulation rates normalized to leaf area increased with crown height and decreased with the age of multi-year old needles. We did not detect a clear latitudinal gradient in foliar Hg accumulation rates.&lt;/p&gt;&lt;p&gt;On an ecosystem scale we developed a simple bottom up approach for foliar Hg(0) uptake considering the systematic variations in crown height, needle age and tree species. We calculated species-specific average foliar Hg(0) dry deposition rates for the 2018 growing season of 22 &amp;#177; 4 &amp;#181;g Hg m&lt;sup&gt;-2&lt;/sup&gt; for beech, 16 &amp;#177; 8 &amp;#181;g Hg m&lt;sup&gt;-2&lt;/sup&gt; for oak, 3 &amp;#177; 0.4 &amp;#181;g Hg m&lt;sup&gt;-2&lt;/sup&gt; for birch, 18 &amp;#177; 10 &amp;#181;g Hg m&lt;sup&gt;-2&lt;/sup&gt; for spruce and 8 &amp;#177; 4 &amp;#181;g Hg m&lt;sup&gt;-2&lt;/sup&gt; for pine. For comparison, the average Hg wet deposition flux measured at 4 of our 10 research sites during the same time period was 2.5 &amp;#177; 0.2 &amp;#181;g Hg m&lt;sup&gt;-2&lt;/sup&gt;.&lt;/p&gt;&lt;p&gt;Scaling up site-specific deposition rates to the forested area of Europe (EU28) resulted in a total aboveground Hg(0) deposition to foliage of approximately 20 Mg during the 2018 growing season. Our results confirm that vegetation uptake of atmospheric Hg(0) represents a major deposition pathway to terrestrial surfaces. The bottom up approach we used is a promising method to quantify Hg(0) deposition fluxes based on easy-to-do Hg concentration measurements in foliage.&lt;/p&gt;


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