scholarly journals Circumpolar transport and air-surface exchange of atmospheric mercury at Ny-Ålesund (79° N), Svalbard, spring 2002

2004 ◽  
Vol 4 (2) ◽  
pp. 1727-1771 ◽  
Author(s):  
J. Sommar ◽  
I. Wängberg ◽  
T. Berg ◽  
K. Gårdfeldt ◽  
J. Munthe ◽  
...  

Abstract. Mercury in different environmental compartments has been measured at Ny-Ålesund (78°54′ N, 11°53′ E) during an intensive campaign, 17 April to 14 May 2002. Time-resolved speciated determination of mercury in the atmosphere and snow was conducted at the Norwegian research station at the Zeppelin mountain, 474 m above the sea level, and at the Italian research facility Dirigibile Italia, 12 m above the sea level. Total Gaseous Mercury (TGM) was present in the range <0.1 to 2.2 ng m−3 during the campaign. Three mercury depletion events, identified as periods with decreased TGM concentrations, were observed. At the lower altitude, TGM concentrations following such events were found to exhibit both higher magnitude and larger variability in comparison to results from the Zeppelin station. Oxidised mercury species in air and fall-out with snow as well as mercury attached to particles were also measured and their concentrations were found to be anti-correlated with TGM in air. The strongest modulation was observed for total mercury concentration (Hg-tot) in snow (range 1.5–76.5 ng L−1). Solid evidence for photo-stimulated emissions of Hg0(g) from the snow pack in conjunction to depletion events were obtained from gradient measurements as well as from flux chamber measurements. Steep diurnal concentration variations of Hg0(aq) in surface seawater were also found to concur with changing solar radiation. The concentration of Hg0(aq) in seawater was found to be in the range 12.2–70.4 pg L−1, which corresponds to supersaturation. Hence, the seawater surface constituted a source emitting elemental mercury. The concentrations of the transient mercury forms RGM (Reactive Gaseous Mercury) and PM (Particulate Mercury) respectively and BrO column densities detected using a zenith and off-axis sky viewing DOAS instrument were very low except for a few individual samples during the major depletion event. An evaluation of trajectories for selected events and comparisons with BrO vertical column densities obtained by the GOME (Global Ozone Monitoring Experiment) instrument aboard the earth remote sensing satellite ESR-2 indicates that the air masses exhibiting low Hg0 concentrations originated from areas with high BrO densities. It was concluded that the observed depletion events at Ny-Ålesund were a results of transport from areas with high photochemical activity around the polar region.

2007 ◽  
Vol 7 (1) ◽  
pp. 151-166 ◽  
Author(s):  
J. Sommar ◽  
I. Wängberg ◽  
T. Berg ◽  
K. Gårdfeldt ◽  
J. Munthe ◽  
...  

Abstract. Mercury in different environmental compartments has been measured at Ny-Ålesund (78°54' N, 11°53' E) during an intensive campaign, 17 April to 14 May 2002. Time-resolved speciated determination of mercury in the atmosphere and snow was conducted at the Norwegian research station at the Zeppelin mountain, 474 m above the sea level, and at the Italian research facility Dirigibile Italia, 12 m above the sea level. Total Gaseous Mercury (TGM) was present in the range <0.1 to 2.2 ng m−3 during the campaign. Three mercury depletion events, identified as periods with decreased TGM concentrations, were observed. At the lower altitude, TGM concentrations following such events were found to exhibit both higher magnitude and larger variability in comparison to results from the Zeppelin station. Oxidised mercury species in air and fall-out with snow as well as mercury attached to particles were also measured and their concentrations were found to be anti-correlated with TGM in air. concentrations of total Hg in snow (Hg-tot) showed a large (~15×) increase in response to Gaseous Elemental Mercury Depletion Events (GEMDEs, range 1.5–76.5 ng L−1). Solid evidence for photo-stimulated emissions of Hg0(g) from the snow pack in conjunction to depletion events were obtained from gradient measurements as well as from flux chamber measurements. Steep diurnal concentration variations of Hg0(aq) in surface seawater were also found to concur with changing solar radiation. The concentration of Hg0(aq) in seawater was found to be in the range 12.2–70.4 pg L−1, which corresponds to supersaturation. Hence, the seawater surface constituted a source emitting elemental mercury. The concentrations of RGM (reactive gaseous mercury), Hg-p (particulate mercury), and BrO column densities (detected by DOAS) were very low except for a few individual samples during the major Hg0 depletion event. BrO vertical column densities obtained by the remote satellite ESR-2 and trajectory analysis indicate that the air masses exhibiting low Hg0 concentrations originated from areas with high BrO densities.


2013 ◽  
Vol 10 (2) ◽  
pp. 102 ◽  
Author(s):  
Andreas Weigelt ◽  
Christian Temme ◽  
Elke Bieber ◽  
Andreas Schwerin ◽  
Maik Schuetze ◽  
...  

Environmental context Mercury is a very hazardous substance for human and environmental health. Systematic long-term direct measurements in the atmosphere can provide valuable information about the effect of emission controls on the global budget of atmospheric mercury, and offer insight into source–receptor transboundary transport of mercury. A complete setup for the measurement of the four most relevant atmospheric mercury species (total gaseous mercury, gaseous oxidised mercury, particle-bound mercury, and gaseous elemental mercury) has been operating at the rural background site of Waldhof, Germany, since 2009. We present the dataset for 2009–2011, the first full-speciation time series for atmospheric mercury reported in Central Europe. Abstract Measurements of mercury species started in 2009 at the air pollution monitoring site ‘Waldhof’ of the German Federal Environmental Agency. Waldhof (52°48′N, 10°45′E) is a rural background site located in the northern German lowlands in a flat terrain, 100km south-east of Hamburg. The temporally highly resolved measurements of total gaseous mercury (TGM), gaseous oxidised mercury (GOM), particle-bound mercury (PBMPM2.5, with particulate matter of a diameter of ≤2.5µm) and gaseous elemental mercury (GEM) cover the period from 2009 to 2011. The complete measurement procedure turned out to be well applicable to detect GOM and PBMPM2.5 levels in the range of 0.4 to 65pgm–3. As the linearity of the analyser was proven to be constant over orders of magnitude, even larger concentrations can be measured accurately. The 3-year median concentration of GEM is found to be 1.61ngm–3, representing typical northern hemispheric background concentrations. With 6.3pgm–3, the 3-year average concentration of PBMPM2.5 is found to be approximately six times higher than the 3-year average GOM concentration. During winter the PBMPM2.5 concentration is on average twice as high as the PBMPM2.5 summer concentration, whereas the GOM concentration shows no clear seasonality. However, on a comparatively low level, a significant diurnal cycle is shown for GOM concentrations. This cycle is most likely related to photochemical oxidation mechanisms. Comparison with selected North American long-term mercury speciation datasets shows that the Waldhof 3-year median speciated mercury data represent typical rural background values.


2008 ◽  
Vol 8 (23) ◽  
pp. 7165-7180 ◽  
Author(s):  
Z.-Q. Xie ◽  
R. Sander ◽  
U. Pöschl ◽  
F. Slemr

Abstract. Atmospheric mercury depletion events (AMDEs) during polar springtime are closely correlated with bromine-catalyzed tropospheric ozone depletion events (ODEs). To study gas- and aqueous-phase reaction kinetics and speciation of mercury during AMDEs, we have included mercury chemistry into the box model MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere), which enables dynamic simulation of bromine activation and ODEs. We found that the reaction of Hg with Br atoms dominates the loss of gaseous elemental mercury (GEM). To explain the experimentally observed synchronous depletion of GEM and O3, the reaction rate of Hg+BrO has to be much lower than that of Hg+Br. The synchronicity is best reproduced with rate coefficients at the lower limit of the literature values for both reactions, i.e. kHg+Br≈3×10−13 and kHg+BrO≤1×10−15 cm3 molecule−1 s−1, respectively. Throughout the simulated AMDEs, BrHgOBr was the most abundant reactive mercury species, both in the gas phase and in the aqueous phase. The aqueous-phase concentrations of BrHgOBr, HgBr2, and HgCl2 were several orders of magnitude larger than that of Hg(SO3)22−. Considering chlorine chemistry outside depletion events (i.e. without bromine activation), the concentration of total divalent mercury in sea-salt aerosol particles (mostly HgCl42−) was much higher than in dilute aqueous droplets (mostly Hg(SO3)22−), and did not exhibit a diurnal cycle (no correlation with HO2 radicals).


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.


Atmosphere ◽  
2019 ◽  
Vol 10 (9) ◽  
pp. 538 ◽  
Author(s):  
James Cizdziel ◽  
Yi Jiang ◽  
Divya Nallamothu ◽  
J. Brewer ◽  
Zhiqiang Gao

Mercury (Hg) is a global pollutant with human health and ecological impacts. Gas exchange between terrestrial surfaces and the atmosphere is an important route for Hg to enter and exit ecosystems. Here, we used a dynamic flux chamber to measure gaseous elemental Hg (GEM) exchange over different landscapes in Mississippi, including in situ measurements for a wetland (soil and water), forest floor, pond, mowed field and grass-covered lawn, as well as mesocosm experiments for three different agricultural soils. Fluxes were measured during both the summer and winter. Mean ambient levels of GEM ranged between 0.93–1.57 ng m−3. GEM emission fluxes varied diurnally with higher daytime fluxes, driven primarily by solar radiation, and lower and more stable nighttime fluxes, dependent mostly on temperature. GEM fluxes (ng m−2 h−1) were seasonally dependent with net emission during the summer (mean 2.15, range 0.32 to 4.92) and net deposition during the winter (−0.12, range −0.32 to 0.12). Total Hg concentrations in the soil ranged from 17.1 ng g−1 to 127 ng g−1 but were not a good predictor of GEM emissions. GEM flux and soil temperature were correlated over the forest floor, and the corresponding activation energy for Hg emission was ~31 kcal mol−1 using the Arrhenius equation. There were significant differences in GEM fluxes between the habitats with emissions for grass > wetland soil > mowed field > pond > wetland water ≈ forest ≈ agriculture soils. Overall, we demonstrate that these diverse landscapes serve as both sources and sinks for airborne Hg depending on the season and meteorological factors.


2016 ◽  
Author(s):  
W. Zhu ◽  
C.-J. Lin ◽  
X. Wang ◽  
J. Sommar ◽  
X. W. Fu ◽  
...  

Abstract. Reliable quantification of air-surfaces flux of elemental Hg vapor (Hg0) is crucial for understanding mercury (Hg) global biogeochemical cycles. There have been extensive measurements and modeling efforts devoting to estimating the exchange fluxes between the atmosphere and various surfaces (e.g., soil, canopies, water, snow, etc.) in past three decades. However, large uncertainty remains due to the complexity of Hg0 bi-directional exchange, limitations of flux quantification techniques and challenges in model parameterization. In this study, we provide a comprehensive review on the state of science in the atmosphere-surface exchange of Hg0. Specifically, the advancement of flux quantification techniques, mechanisms in driving the air-surfaces Hg exchange, and modeling efforts are presented. Due to the semi-volatile nature of Hg0 and redox transformation of Hg in environmental media, Hg deposition and evasion are influenced by multiple environmental variables including seasonality, vegetative coverage and its life cycle, temperature, light, moisture, atmospheric turbulence, presence of reactants (e.g., O3, radicals, etc.) that drives the physicochemical process of Hg in the media where Hg0 exchange occurs. However, effects of these processes on flux have not been fundamentally and quantitatively determined, which limits the accuracy of flux modeling. In this study, we compile an up-to-date global observational flux database and discuss the implication of flux data on global Hg budget. Mean Hg0 flux obtained by micrometeorological measurement did not appear to be significantly greater than the flux measured by dynamic flux chamber methods over unpolluted surfaces (p=0.16, one-tailed, Mann-Whitney U test). The spatio-temporal coverage of existing Hg0 flux measurements is highly heterogeneous with large data gaps existing in multiple continents (Africa, South Asia, Middle East, South America and Australia). The magnitude of evasion flux is strongly enhanced by human activities, particularly at contaminated sites. Hg0 flux observations in East Asia are comparatively larger in magnitude than the rest of the world, suggesting substantial reemission of previously deposited mercury from anthropogenic sources. Hg0 exchange over pristine surfaces (e.g., background soil and water) and vegetation need better constrains for global analysis of atmospheric Hg budget. The existing knowledge gap and the associated research needs for future measurements and modeling efforts for the air-surface exchange of Hg0 are discussed.


2017 ◽  
Author(s):  
Dean Howard ◽  
Grant C. Edwards

Abstract. Aerodynamic gradient measurements of the air–surface exchange of gaseous elemental mercury (GEM) were undertaken over a 40 hectare alpine grassland in Australia's Snowy Mountains region during the austral summer. Bi-directional GEM fluxes were observed throughout the study, with overall mean value of 0.2 ± 14.8 ng m-2 h-1 and mean nocturnal fluxes of −1.5 ± 7.8 ng m-2 h-1 compared to diurnal fluxes of 1.8 ± 18.6 ng m-2 h-1. Deposition velocities ranged from −2.2 cm s-1 to 2.9 cm s-1, whilst ambient GEM concentrations throughout the study were 0.59 ± 0.10 ng m-3. Cumulative GEM fluxes correlated well with 24-hour running mean soil temperatures, and one precipitation event was shown to have a positive impact on diurnal emission fluxes. The underlying vegetation had largely senesced and showed little stomatal control on fluxes. Nocturnal atmospheric mercury depletion events (NAMDEs) were observed concomitant with O3 depletion and dew formation under shallow, stable nocturnal boundary layers. A mass balance box model was able to reproduce ambient GEM concentration patterns during NAMDE and non-NAMDE nights without invoking chemical oxidation of GEM throughout the column, indicating the role of surface processes controlling deposition in these events. Surface deposition was enhanced under NAMDE nights, though uptake to dew likely represents less than one fifth of this enhanced deposition. Instead, enhancement of the surface GEM gradient as a result of oxidation at the surface in the presence of dew is hypothesised to be responsible for a large portion of GEM depletion during these particular events. GEM emission pulses following nights with significant deposition provide evidence for the prompt recycling of 17 % of deposited mercury, with the remaining portion retained in surface sinks. The long-term impacts of any sinks are however likely to be minimal, as cumulative GEM flux across the 3-week study period was close to zero.


2013 ◽  
Vol 13 (10) ◽  
pp. 5325-5336 ◽  
Author(s):  
G. C. Edwards ◽  
D. A. Howard

Abstract. This paper presents the first gaseous elemental mercury (GEM) air-surface exchange measurements obtained over naturally enriched and background (<0.1 μg g−1 Hg) terrestrial landscapes in Australia. Two pilot field studies were carried out during the Australian autumn and winter periods at a copper-gold-cobalt-arsenic-mercury mineral field near Pulganbar, NSW. GEM fluxes using a dynamic flux chamber approach were measured, along with controlling environmental parameters over three naturally enriched and three background substrates. The enriched sites results showed net emission to the atmosphere and a strong correlation between flux and substrate Hg concentration, with average fluxes ranging from 14 ± 1 ng m−2 h−1 to 113 ± 6 ng m−2 h−1. Measurements at background sites showed both emission and deposition. The average Hg flux from all background sites showed an overall net emission of 0.36 ± 0.06 ng m−2 h−1. Fluxes show strong relationships with temperature, radiation, and substrate parameters. A compensation point of 2.48, representative of bare soils was determined. For periods of deposition, dry deposition velocities ranged from 0.00025 cm s−1 to 0.0083 cm s−1 with an average of 0.0041 ± 0.00018 cm s−1, representing bare soil, nighttime conditions. Comparison of the Australian data to North American data suggests the need for Australian-specific mercury air-surface exchange data representative of Australia's unique climatic conditions, vegetation types, land use patterns and soils.


2018 ◽  
Vol 18 (1) ◽  
pp. 129-142 ◽  
Author(s):  
Dean Howard ◽  
Grant C. Edwards

Abstract. Aerodynamic gradient measurements of the air–surface exchange of gaseous elemental mercury (GEM) were undertaken over a 40 ha alpine grassland in Australia's Snowy Mountains region across a 3-week period during the late austral summer. Bi-directional GEM fluxes were observed throughout the study, with overall mean value of 0.2 ± 14.5 ng m−2 h−1 and mean nocturnal fluxes of −1.5 ± 7.8 ng m−2 h−1 compared to diurnal fluxes of 1.8 ± 18.6 ng m−2 h−1. Deposition velocities ranged from −2.2 to 2.9 cm s−1, whilst ambient GEM concentrations throughout the study were 0.59 ± 0.10 ng m−3. Cumulative GEM fluxes correlated well with 24 h running mean soil temperatures, and one precipitation event was shown to have a positive impact on diurnal emission fluxes. The underlying vegetation had largely senesced and showed little stomatal control on fluxes. Nocturnal atmospheric mercury depletion events (NAMDEs) were observed concomitant with O3 depletion and dew formation under shallow, stable nocturnal boundary layers. A mass balance box model was able to reproduce ambient GEM concentration patterns during NAMDE and non-NAMDE nights without invoking chemical oxidation of GEM throughout the column, indicating a significant role of surface processes controlling deposition in these events. Surface deposition was enhanced under NAMDE nights, though uptake to dew likely represents less than one-fifth of this enhanced deposition. Instead, enhancement of the surface GEM gradient as a result of oxidation at the surface in the presence of dew is hypothesised to be responsible for a large portion of GEM depletion during these particular events. GEM emission pulses following nights with significant deposition provide evidence for the prompt recycling of 17 % of deposited mercury, with the remaining portion retained in surface sinks. The long-term impacts of any sinks are however likely to be minimal, as cumulative GEM flux across the study period was close to zero.


2008 ◽  
Vol 8 (4) ◽  
pp. 13197-13232 ◽  
Author(s):  
Z.-Q. Xie ◽  
R. Sander ◽  
U. Pöschl ◽  
F. Slemr

Abstract. Atmospheric mercury depletion events (AMDEs) during polar springtime are closely correlated with bromine-catalyzed tropospheric ozone depletion events (ODEs). To study gas- and aqueous-phase reaction kinetics and speciation of mercury during AMDEs, we have included mercury chemistry into the box model MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere), which enables dynamic simulation of bromine activation and ODEs. We found that the reaction of Hg with Br atoms dominates the loss of gaseous elemental mercury (GEM). To explain the experimentally observed synchronous destruction of Hg and O3, the reaction rate of Hg+BrO has to be much lower than that of Hg+Br. The synchronicity is best reproduced with rate coefficients at the lower limit of the literature values for both reactions, i.e. kHg+Br≈3×10-13 and kHg+BrO≤1×10-15cm3 mol-1 s-1, respectively. Throughout the simulated AMDEs, BrHgOBr was the most abundant reactive mercury species, both in the gas phase and in the aqueous phase. The aqueous phase concentrations of BrHgOBr, HgBr2, and HgCl2 were several orders of magnitude larger than that of Hg(SO3)2-2. Considering chlorine chemistry outside depletion events (i.e. without bromine activation), the concentration of total divalent mercury in sea-salt aerosol particles (mostly HgCl2) was much higher than in dilute aqueous droplets (mostly Hg(SO3)2-2), and did not exhibit a diurnal cycle (no correlation with HO2 radicals).


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