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).

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 Investigation of processes controlling summertime gaseous elemental mercury oxidation at midlatitudinal marine, coastal, and inland sites

2016 ◽  
Vol 16 (13) ◽  
pp. 8461-8478 ◽  
Author(s):  
Zhuyun Ye ◽  
Huiting Mao ◽  
Che-Jen Lin ◽  
Su Youn Kim
Keyword(s):  
Marine Boundary Layer ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Box Model ◽  
Chemical Mechanism ◽  
Gaseous Elemental Mercury ◽  
Diurnal Cycles ◽  
Mixing Ratios ◽  
Halogen Chemistry ◽  
Marine Site

Abstract. A box model incorporating a state-of-the-art chemical mechanism for atmospheric mercury (Hg) cycling was developed to investigate the oxidation of gaseous elemental mercury (GEM) at three locations in the northeastern United States: Appledore Island (AI; marine), Thompson Farm (TF; coastal, rural), and Pack Monadnock (PM; inland, rural, elevated). The chemical mechanism in this box model included the most up-to-date Hg and halogen chemistry. As a result, the box model was able to simulate reasonably the observed diurnal cycles of gaseous oxidized mercury (GOM) and chemical speciation bearing distinct differences between the three sites. In agreement with observations, simulated GOM diurnal cycles at AI and TF showed significant daytime peaks in the afternoon and nighttime minimums compared to flat GOM diurnal cycles at PM. Moreover, significant differences in the magnitude of GOM diurnal amplitude (AI > TF > PM) were captured in modeled results. 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) atmosphere, Br and BrO became dominant GEM oxidants, with mixing ratios reaching 0.1 and 1 pptv, respectively, and contributing ∼ 70 % of the total GOM production during midday, while O3 dominated GEM oxidation (50–90 % of GOM production) over the remaining day when Br and BrO mixing ratios were diminished. The majority of HgBr produced from GEM+Br was oxidized by NO2 and HO2 to form brominated GOM species. Relative humidity and products of the CH3O2+BrO reaction possibly significantly affected the mixing ratios of Br or BrO radicals and subsequently GOM formation. Gas–particle partitioning could potentially be important in the production of GOM as well as Br and BrO at the marine site.

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 A 2 year record of atmospheric mercury species at a background Southern Hemisphere station on Amsterdam Island

2014 ◽  
Vol 14 (10) ◽  
pp. 14439-14470
Author(s):  
H. Angot ◽  
M. Barret ◽  
O. Magand ◽  
M. Ramonet ◽  
A. Dommergue
Keyword(s):  
Indian Ocean ◽  
Southern Hemisphere ◽  
Marine Boundary Layer ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Southern Indian Ocean ◽  
Observation System ◽  
Mercury Species ◽  
Back Trajectories ◽  
Gaseous Elemental Mercury

Abstract. Scarcity of mercury species records in the Southern Hemisphere is a critical weak point for the development of appropriate modeling and regulation scenarios. Under the framework of the "Global Mercury Observation System" (GMOS) project, a monitoring station has been set up on Amsterdam Island (37°48' S, 77°34' E) in the remote southern Indian Ocean. For the first time in the Southern Hemisphere, a 2 year record of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) is presented. GEM concentrations were remarkably steady (1.03 ± 0.08 pg m−3) while RGM and PBM concentrations were very low and exhibited a strong variability (mean: 0.34 pg m−3 [range: 0.28–4.07 pg m−3] and mean: 0.67 pg m−3 [range: 0.28–12.67 pg m−3], respectively). Despite the remoteness of the island, wind sector analysis, air mass back trajectories and the observation of radonic storms highlighted a long-range contribution from the southern African continent to the GEM and PBM budgets in winter during the biomass burning season. Lowest concentrations of GEM were associated with southerly polar and marine air masses from the remote southern Indian Ocean. This unique dataset provides new baseline GEM concentrations in the Southern Hemisphere mid-latitudes for further modeling studies, while mercury speciation along with upcoming wet deposition data will help improving our understanding of mercury cycle in the marine boundary layer.

Reproducing polar springtime bromine explosion events, ozone depletion events and atmospheric mercury depletion events in an outdoor mesocosm sea-ice facility

2021 ◽  
Author(s):  
Zhiyuan Gao ◽  
Feiyue Wang ◽  
Nicolas-Xavier Geilfus
Keyword(s):  
Sea Ice ◽  
Ozone Depletion ◽  
Polar Region ◽  
Surface Ozone ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Environmental Research ◽  
The Arctic ◽  
Gaseous Elemental Mercury ◽  
Air Temperatures

<p>Every year during polar sunrise, a series of photochemical events are observed episodically in the troposphere over the Arctic and Antarctic, including bromine explosion events (BEEs), ozone depletion events (ODEs), and mercury depletion events (MDEs). Extensive studies show that all these events are triggered by gas-phase reactive bromine species that are photochemically activated from sea-salt bromide via multi-phase reactions under freezing air temperatures. However, major knowledge gaps exist in both fundamental cryo-photochemical processes and local meteorological conditions that may affect the timing and magnitude of those events. Here, we present an outdoor mesocosm-scale experiment in which we studied the depletion of surface ozone and gaseous elemental mercury at the Sea-ice Environmental Research Facility (SERF) in Winnipeg, Canada, in an urban and non-polar region. Temporal changes in ozone and gaseous elemental mercury concentrations inside acrylic tubes were monitored over bromide-enriched artificial seawater during entire sea ice freeze-and-melt cycles and open water periods. Mid-day photochemical loss of both gas species was observed in the boundary layer air immediately above the sea ice surface, in a pattern that is characteristic of BEE-induced ODEs and MDEs in the Arctic. The importance of UV radiation and sea ice presence in causing such observations was demonstrated by sampling from UV-transmitting and UV-blocking acrylic tubes under different air temperatures. The ability of reproducing mesocosm-scale BEE-induced ODEs and MDEs in a non-polar region provides a new platform with opportunities to systematically study the cryo-photochemical mechanisms leading to BEEs, ODEs, and MDEs in the Arctic, their role in biogeochemical cycles across the ocean-sea ice-atmosphere interfaces, and their sensitivities to a changing climate. </p>

Towards an advanced description and modelling of the atmospheric multiphase chemistry of mercury: CAPRAM HG module 1.0

2021 ◽  
Author(s):  
Erik Hans Hoffmann ◽  
Tao Li ◽  
Andreas Tilgner ◽  
Yan Wang ◽  
Hartmut Herrmann
Keyword(s):  
Gas Phase ◽  
Aqueous Phase ◽  
Aerosol Particles ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Gas Phase Reactions ◽  
Gaseous Elemental Mercury ◽  
Gas Phase Chemistry ◽  
Reactive Halogen Species ◽  
Phase Chemistry

<p>Mercury is a neurotoxic element emitted predominantly in its less-reactive form as gaseous elemental mercury (GEM) into the atmosphere by various natural and anthropogenic processes. Once emitted it undergoes chemical processing in the atmospheric gas and aqueous phase. There, GEM is oxidised into gaseous oxidised mercury (GOM), which partitions into aerosol particles residing there as particulate bounded mercury (PBM) due to its much higher solubility. The faster deposition of GOM and PBM compared to GEM is of special environmental importance, because they can be converted into more toxic organic mercury in aquatic environments and then take serious place in the food web. Thus, it is crucial for models to understand the transformation of GEM into GOM and PBM and vice versa. To date, numerous gas-phase chemistry simulations were performed, but reveal missing oxidation and reduction processes. However, only few models exist that investigate the multiphase mercury chemistry in a detailed manner.</p><p>Therefore, a comprehensive multiphase mercury chemistry mechanism, the CAPRAM HG module 1.0 (CAPRAM-HG1.0), has been developed. The CAPRAM-HG1.0 includes 74 gas-phase reactions, 22 phase transfers and 77 aqueous-phase reactions. It was coupled to the multiphase chemistry mechanism MCMv3.2/CAPRAM4.0 and the extended CAPRAM halogen module 3.0 (CAPRAM-HM3.0) for investigations of multiphase Hg redox under Chinese polluted conditions. Simulations were performed for summer conditions in 2014 using the air parcel model SPACCIM to investigate the performance of the model to simulate typical concentrations and patterns of GEM, GOM and PBM.</p><p>Under non-cloud conditions, model results reveal good coincides with concentrations and patterns for GEM, GOM and PBM measured in China. However, the simulations also show that there are still high uncertainties in atmospheric mercury chemistry. Especially, the complexation with HULIS within aerosol particles needs evaluation as the simulations indicate this process as key process driving concentrations and patterns of both GOM and PBM. Further, the present study demonstrates the need of a better understanding of continental concentrations of reactive halogen species and particle bounded halides as well as their link to the multiphase chemistry and atmospheric cycling of mercury.</p>

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 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 Natural and anthropogenic atmospheric mercury in the European Arctic: a speciation study

2010 ◽  
Vol 10 (11) ◽  
pp. 27255-27281
Author(s):  
A. O. Steen ◽  
T. Berg ◽  
A. P. Dastoor ◽  
D. A. Durnford ◽  
L. R. Hole ◽  
...  
Keyword(s):  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Mercury Species ◽  
In Situ Oxidation ◽  
Air Masses ◽  
Gaseous Elemental Mercury ◽  
Complete Dataset ◽  
Speciation Study ◽  
European Arctic

Abstract. It is agreed that gaseous elemental mercury (GEM) is converted to reactive gaseous mercury (RGM) during springtime Atmospheric Mercury Depletion Event (AMDE). RGM is associated with aerosols (PHg) provided that there are sufficient aerosols available for the conversion from RGM to PHg to occur. This study reports the longest time series of GEM, RGM and PHg concentrations from a European Arctic site. From 27 April 2007 until 31 December 2008 composite GEM, RGM and PHg measurements were conducted in Ny-Ålesund (78°54' N, 11°53' E). The average concentrations of the complete dataset were 1.62±0.3 ng m−3, 8±13 pgm−3 and 8±25 pgm−3 for GEM, RGM and PHg, respectively. The study revealed a clear seasonal distribution of GEM, RGM and PHg previously undiscovered. For the complete dataset the atmospheric mercury distribution was 99% GEM, whereas RGM and PHg constituted <1%. Increased PHg concentration occurred exclusively from March through April, and constituted on average 75% of the reactive mercury species in the respective period. RGM was suggested as the precursor for the PHg existence, but long range transportation of PHg has to be taken into consideration. Surprisingly, RGM was not solely formed during the spring AMDE season. Environment Canada's Global/Regional Atmospheric Heavy Metal model (GRAHM) suggested that in situ oxidation of GEM by ozone may be producing the increased RGM concentrations from March through August. Most likely, in situ oxidation of GEM by BrO produced the observed RGM from March through August. The AMDEs occurred from late March until mid June and were thought to be of non-local origin, with GEM being transported to the study site by a wide variety of air masses. With some exceptions, no clear meteorological regime was associated with the GEM, RGM and PHg concentrations.

scholarly journals Speciated Atmospheric Mercury during Haze and Non-haze Days in an Inland City in China

2016 ◽  
Author(s):  
Qianqian Hong ◽  
Zhouqing Xie ◽  
Cheng Liu ◽  
Feiyue Wang ◽  
Pinhua Xie ◽  
...  
Keyword(s):  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Central China ◽  
Mercury Emissions ◽  
Gaseous Elemental Mercury ◽  
Enhanced Production ◽  
Mercury Transport ◽  
Haze Pollution ◽  
The Mean ◽  
Haze Days

Abstract. Long-term continuous measurements of speciated atmospheric mercury were conducted at Hefei, a mid-latitude inland city in east central China, from July 2013 to June 2014. The mean concentrations (± standard deviation) of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) were 3.95 ± 1.93 ng m−3, 2.49 ± 2.41 pg m−3 and 23.3 ± 90.8 pg m−3, respectively, during non-haze days, and 4.74 ± 1.62 ng m−3, 4.32 ± 8.36 pg m−3 and 60.2 ± 131.4 pg m−3, respectively, during haze days. Potential source contribution function (PSCF) analysis suggested that the atmospheric mercury pollution during haze days was caused primarily by local mercury emissions, instead of via long-range mercury transport. In addition, the disadvantageous diffussion during haze days will also enhance the level of atmospheric mercury. Compared to the GEM and RGM, change in PBM was more sensitive to the haze pollution. The mean PBM concentration during haze days was 2.5 times that during non-haze days due to elevated concentrations of particulate matter. A remarkable seasonal trend in PBM was observed with concentration decreasing in the following order in response to the frequency of haze days: autumn, winter, spring, summer. A distinct diurnal relationship was found between GEM and RGM during haze days, with the peak values of RGM coinciding with the decline in GEM. Using HgOH as an intermediate product during GEM oxidation, our results suggest that NO2 aggregation with HgOH could explain the enhanced production of RGM during the daytime in haze days. Increasing level of NOx will potentially accelerate the oxidation of GEM despite the decrease of solar radiation.

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