scholarly journals Measurements of atmospheric mercury species at a German rural background site from 2009 to 2011 – methods and results

2013 ◽  
Vol 10 (2) ◽  
pp. 102 ◽  
Author(s):  
Andreas Weigelt ◽  
Christian Temme ◽  
Elke Bieber ◽  
Andreas Schwerin ◽  
Maik Schuetze ◽  
...  
Keyword(s):  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Pollution Monitoring ◽  
Mercury Species ◽  
Total Gaseous Mercury ◽  
Gaseous Elemental Mercury ◽  
Rural Background ◽  
Background Site ◽  
Gaseous Mercury

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.

scholarly journals Simulation of atmospheric mercury depletion events (AMDEs) during polar springtime using the MECCA box model

2008 ◽  
Vol 8 (23) ◽  
pp. 7165-7180 ◽  
Author(s):  
Z.-Q. Xie ◽  
R. Sander ◽  
U. Pöschl ◽  
F. Slemr
Keyword(s):  
Aqueous Phase ◽  
Ozone Depletion ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Box Model ◽  
Rate Coefficients ◽  
Mercury Species ◽  
Phase Reaction ◽  
Gaseous Elemental Mercury ◽  
Sea Salt Aerosol

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).

Gaseous mercury in coastal urban areas

2010 ◽  
Vol 7 (6) ◽  
pp. 537 ◽  
Author(s):  
Anne L. Soerensen ◽  
Henrik Skov ◽  
Matthew S. Johnson ◽  
Marianne Glasius
Keyword(s):  
Urban Areas ◽  
Marine Boundary Layer ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Mercury Deposition ◽  
Mercury Emissions ◽  
Gaseous Elemental Mercury ◽  
Gaseous Mercury ◽  
Range Transport ◽  
Aquatic Food

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.

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

2007 ◽  
Vol 7 (1) ◽  
pp. 151-166 ◽  
Author(s):  
J. Sommar ◽  
I. Wängberg ◽  
T. Berg ◽  
K. Gårdfeldt ◽  
J. Munthe ◽  
...  
Keyword(s):  
Sea Level ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Mercury Species ◽  
Research Station ◽  
Flux Chamber ◽  
Vertical Column ◽  
Surface Exchange ◽  
Lower Altitude ◽  
Gaseous Mercury

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.

scholarly journals Simulation of atmospheric mercury depletion events (AMDEs) during polar springtime using the MECCA box model

2008 ◽  
Vol 8 (4) ◽  
pp. 13197-13232 ◽  
Author(s):  
Z.-Q. Xie ◽  
R. Sander ◽  
U. Pöschl ◽  
F. Slemr
Keyword(s):  
Aqueous Phase ◽  
Ozone Depletion ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Box Model ◽  
Rate Coefficients ◽  
Mercury Species ◽  
Phase Reaction ◽  
Gaseous Elemental Mercury ◽  
Sea Salt Aerosol

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).

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 ◽  
...  
Keyword(s):  
Sea Level ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Mercury Species ◽  
Research Station ◽  
Flux Chamber ◽  
Vertical Column ◽  
Surface Exchange ◽  
Lower Altitude ◽  
Gaseous Mercury

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.

scholarly journals A Local Scale Modeling Study of Mercury Depletion Event at Canadian Arctic

2021 ◽  
Author(s):  
Minish Panchall
Keyword(s):  
Measurement Data ◽  
Canadian Arctic ◽  
Elemental Mercury ◽  
Local Scale ◽  
Atmospheric Mercury ◽  
Scale Model ◽  
Mercury Species ◽  
Time Step ◽  
Gaseous Elemental Mercury ◽  
Modeling Study

A modeling study was conducted on the transformation and deposition patterns of atmospheric mercury in the Canadian Arctic. One Dimensional (1-D) local scale model was used to simulate the episodic depletions of gaseous elemental mercury (GEM) after polar sunrise at Alert, Canada. The model was developed by starting with existing meteorological model (LCM-Local Climate Model) which is coupled with Canadian Aerosol Module (CAM) and then adding modules specific to atmospheric mercury chemistry. The model is able to simulate local scale transport of mercury over the entire depth of the troposphere with a basic time step of 20 min. and incorporates current knowledge of transformation reactions of atmospheric mercury species. Three mercury species Hg(O), Hg(II) and Hg(p) were considered. The developed model was applied to a portion of the Canadian Arctic region, Alert, for the month of April 2002. The model was then evaluated by comparing model estimates of mercury species concentrations with the measurement data collected in the Canadian Arctic by Meteorological Services of Canada, Downsview, Ontario. The results from this modeling study agree reasonably well with some underestimation caused by lower conversion of gaseous elemental mercury (GEM) into reactive gaseous mercury (RGM) and subsequent conversion to total particulate mercury (TPM). A sensitivity analysis was also conducted to examine the depositions of mercury species in response to changes in ozone and soot concentrations.

scholarly journals Two new sources of reactive gaseous mercury in the free troposphere

2012 ◽  
Vol 12 (11) ◽  
pp. 29203-29233 ◽  
Author(s):  
H. Timonen ◽  
J. L. Ambrose ◽  
D. A. Jaffe
Keyword(s):  
Source Region ◽  
Elemental Mercury ◽  
Anthropogenic Pollution ◽  
Atmospheric Mercury ◽  
Free Troposphere ◽  
Mercury Deposition ◽  
Gaseous Elemental Mercury ◽  
Reactive Gaseous Mercury ◽  
Gaseous Mercury ◽  
The Pacific

Abstract. Mercury (Hg) is a neurotoxin that bioaccumulates in the food chain. Mercury is emitted to the atmosphere primarily in its elemental form, which has a long lifetime allowing global transport. It is known that atmospheric oxidation of gaseous elemental mercury (GEM) generates reactive gaseous mercury (RGM) which plays an important role in the atmospheric mercury cycle by enhancing the rate of mercury deposition to ecosystems. However, the primary GEM oxidants, and the sources and chemical composition of RGM are poorly known. Using speciated mercury measurements conducted at the Mt. Bachelor Observatory since 2005 we present two previously unidentified sources of RGM to the free troposphere (FT). Firstly, we observed elevated RGM concentrations, large RGM/GEM-ratios, and anti-correlation between RGM and GEM during Asian long-rang transport events, demonstrating that RGM is formed from GEM by in-situ oxidation in some anthropogenic pollution plumes in the FT. During the Asian pollution events the measured RGM/GEM-ratios reached peak values, up to ~0.20, which are significantly larger than ratios typically measured (RGM/GEM < 0.05) in the Asian source region. Secondly, we observed very high RGM levels – the highest reported in the FT – in clean air masses that were processed upwind of Mt. Bachelor Observatory over the Pacific Ocean. The high RGM concentrations (up to 700 pg m−3), high RGM/GEM-ratios (up to 1), and very low ozone levels during these events provide the first observational evidence indicating significant GEM oxidation in the lower FT. The identification of these processes changes our conceptual understanding of the formation and distribution of oxidized Hg in the global atmosphere.

scholarly journals In-situ and Denuder Based Measurements of Elemental and Reactive Gaseous Mercury with Analysis by Laser-Induced Fluorescence. Results from the Reno Atmospheric Mercury Intercomparison Experiment

2016 ◽  
Author(s):  
Anthony J. Hynes ◽  
Stephanie Everhart ◽  
Dieter Bauer ◽  
James Remeika ◽  
Cheryl Tatum Ernest
Keyword(s):  
Single Photon ◽  
Thermal Dissociation ◽  
Elemental Mercury ◽  
Laser Induced Fluorescence ◽  
Atmospheric Mercury ◽  
Substantial Contribution ◽  
Gaseous Elemental Mercury ◽  
Gaseous Mercury ◽  
The University

Abstract. The University of Miami (UM) deployed a sequential two photon laser-induced fluorescence (2P-LIF) instrument for the in-situ measurement of gaseous elemental mercury, Hg(0), during the Reno Atmospheric Mercury Intercomparison Experiment (RAMIX) campaign. A number of extended sampling experiments, typically lasting 6–8 hours but on one occasion extending to ~ 24 hours, were conducted allowing the 2P-LIF measurements of Hg(0) concentrations to be compared with two independently operated instruments using gold amalgamation sampling coupled with Cold Vapor Atomic Fluorescence Spectroscopic (CVAFS) analysis. At the highest temporal resolution, ~ 5 minute samples, the three instruments measured concentrations that agreed to within 10–25 %. Measurements of total gaseous mercury (TGM) were made by using pyrolysis to convert total oxidized mercury (TOM) to Hg(0). TOM was then obtained by difference. Variability in the ambient Hg(0) concentration limited our sensitivity for measurement of ambient TOM using this approach. In addition, manually sampled KCl coated annular denuders were deployed and analyzed using thermal dissociation coupled with single photon LIF detection of Hg(0). The TOM measurements obtained were normally consistent with KCl denuder measurements obtained with two Tekran speciation systems and with the manual KCl denuder measurements but with very large uncertainty. They were typically lower than measurements reported by the University of Washington (UW) Detector for Oxidized Hg Species (DOHGS) system. The ability of the 2P-LIF pyrolysis system to measure TGM was demonstrated during one of the manifold HgBr2 spikes but the results did not agree well with those reported by the DOHGS system. We suggest that instrumental artifacts make a substantial contribution to the discrepancies in the reported measurements over the course of the RAMIX campaign. This suggests that caution should be used in drawing significant implications for the atmospheric cycling of mercury.

scholarly journals Trend of atmospheric mercury concentrations at Cape Point for 1995–2004 and since 2007

2017 ◽  
Vol 17 (3) ◽  
pp. 2393-2399 ◽  
Author(s):  
Lynwill G. Martin ◽  
Casper Labuschagne ◽  
Ernst-Günther Brunke ◽  
Andreas Weigelt ◽  
Ralf Ebinghaus ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Wet Deposition ◽  
Southern Oscillation ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Austral Spring ◽  
Mercury Emissions ◽  
Gaseous Elemental Mercury ◽  
Regional Processes

Abstract. Long-term measurements of gaseous elemental mercury (GEM) concentrations at Cape Point, South Africa, reveal a downward trend between September 1995 and December 2005 and an upward one from March 2007 until June 2015, implying a change in trend sign between 2004 and 2007. The trend change is qualitatively consistent with the trend changes in GEM concentrations observed at Mace Head, Ireland, and in mercury wet deposition over North America, suggesting a change in worldwide mercury emissions. Seasonally resolved trends suggest a modulation of the overall trend by regional processes. The trends in absolute terms (downward in 1995–2004 and upward in 2007–2015) are highest in austral spring (SON), coinciding with the peak in emissions from biomass burning in South America and southern Africa. The influence of trends in biomass burning is further supported by a biennial variation in GEM concentration found here and an El Niño–Southern Oscillation (ENSO) signature in GEM concentrations reported recently.

scholarly journals Trend of atmospheric mercury concentrations at Cape Point for 1995–2004 and since 2007

2016 ◽  
Author(s):  
Lynwill G. Martin ◽  
Casper Labuschagne ◽  
Ernst-Günther Brunke ◽  
Andreas Weigelt ◽  
Ralf Ebinghaus ◽  
...  
Keyword(s):  
South Africa ◽  
Biomass Burning ◽  
Wet Deposition ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Austral Spring ◽  
Mercury Emissions ◽  
Gaseous Elemental Mercury ◽  
Regional Processes

Abstract. Long-term measurements of gaseous elemental mercury (GEM) concentrations at Cape Point, South Africa, reveal a downward trend between September 1995 and December 2005 and an upward one since March 2007 until June 2015 implying a change in trend sign between 2004 and 2007. The trend change is qualitatively consistent with the trend changes in GEM concentrations observed at Mace Head, Ireland, and in mercury wet deposition over North America suggesting a change in worldwide mercury emissions. Seasonally resolved trends suggest a modulation of the overall trend by regional processes. The trends in absolute terms (downward in 1995–2004 and upward in 2007–2015) are the highest in austral spring (SON) coinciding with the peak in emissions from biomass burning in South America and southern Africa. The influence of trends in biomass burning is further supported by a biennial variation in GEM concentration found here and an ENSO signature in GEM concentrations reported recently.

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