scholarly journals Nested-grid simulation of mercury over North America

2012 ◽  
Vol 12 (1) ◽  
pp. 2603-2646 ◽  
Author(s):  
Y. Zhang ◽  
L. Jaeglé ◽  
A. van Donkelaar ◽  
R. V. Martin ◽  
C. D. Holmes ◽  
...  
Keyword(s):  
North America ◽  
Wet Deposition ◽  
Transport Model ◽  
Atmospheric Mercury ◽  
Anthropogenic Emissions ◽  
Spatial And Temporal Variability ◽  
Deposition Flux ◽  
Nested Model ◽  
The Us ◽  
Nested Grid

Abstract. We have developed a new high-resolution (1/2° latitude by 2/3° longitude) nested-grid mercury (Hg) simulation over North America employing the GEOS-Chem global chemical transport model. Emissions, chemistry, deposition, and meteorology are self-consistent between the global and nested domains. Compared to the global model (4° latitude by 5° longitude), the nested model shows improved skill at capturing the high spatial and temporal variability of Hg wet deposition over North America observed by the Mercury Deposition Network (MDN) in 2008–2009. The nested simulation resolves features such as land/ocean contrast and higher deposition due to orographic precipitation, and predicts more efficient convective rain scavenging of Hg over the southeast United States. However, the nested model overestimates Hg wet deposition over the Ohio River Valley region (ORV) by 27%. We modify anthropogenic emission speciation profiles in the US EPA National Emission Inventory (NEI) to account for the rapid in-plume reduction of reactive to elemental Hg (IPR simulation). This leads to a decrease in the model bias to +3% over the ORV region. Over the contiguous US, the correlation coefficient (r) between MDN observations and our IPR simulation increases from 0.63 to 0.78. The IPR nested simulation generally reproduces the seasonal cycle in surface concentrations of speciated Hg from the Atmospheric Mercury Network (AMNet) and Canadian Atmospheric Mercury Network (CAMNet). In the IPR simulation, annual mean reactive gaseous and particulate-bound Hg are within 80% and 10% of observations, respectively. In contrast, the simulation with unmodified anthropogenic Hg speciation profiles overestimates these observations by factors of 2 to 4. The nested model shows improved skill at capturing the horizontal variability of Hg observed over California during the ARCTAS aircraft campaign. We find that North American anthropogenic emissions account for 10–22% of Hg wet deposition flux over the US, depending on the anthropogenic emissions speciation profile assumed. The percent contribution can be as high as 60% near large point emission sources in ORV. The contribution for the dry deposition is 13–20%.

scholarly journals Nested-grid simulation of mercury over North America

2012 ◽  
Vol 12 (14) ◽  
pp. 6095-6111 ◽  
Author(s):  
Y. Zhang ◽  
L. Jaeglé ◽  
A. van Donkelaar ◽  
R. V. Martin ◽  
C. D. Holmes ◽  
...  
Keyword(s):  
North America ◽  
North American ◽  
Wet Deposition ◽  
Atmospheric Mercury ◽  
Point Sources ◽  
Anthropogenic Emissions ◽  
Spatial And Temporal Variability ◽  
Nested Model ◽  
The Us ◽  
Nested Grid

Abstract. We have developed a new nested-grid mercury (Hg) simulation over North America with a 1/2° latitude by 2/3° longitude horizontal resolution employing the GEOS-Chem global chemical transport model. Emissions, chemistry, deposition, and meteorology are self-consistent between the global and nested domains. Compared to the global model (4° latitude by 5° longitude), the nested model shows improved skill at capturing the high spatial and temporal variability of Hg wet deposition over North America observed by the Mercury Deposition Network (MDN) in 2008–2009. The nested simulation resolves features such as higher deposition due to orographic precipitation, land/ocean contrast and and predicts more efficient convective rain scavenging of Hg over the southeast United States. However, the nested model overestimates Hg wet deposition over the Ohio River Valley region (ORV) by 27%. We modify anthropogenic emission speciation profiles in the US EPA National Emission Inventory (NEI) to account for the rapid in-plume reduction of reactive to elemental Hg (IPR simulation). This leads to a decrease in the model bias to −2.3% over the ORV region. Over the contiguous US, the correlation coefficient (r) between MDN observations and our IPR simulation increases from 0.60 to 0.78. The IPR nested simulation generally reproduces the seasonal cycle in surface concentrations of speciated Hg from the Atmospheric Mercury Network (AMNet) and Canadian Atmospheric Mercury Network (CAMNet). In the IPR simulation, annual mean gaseous and particulate-bound Hg(II) are within 140% and 11% of observations, respectively. In contrast, the simulation with unmodified anthropogenic Hg speciation profiles overestimates these observations by factors of 4 and 2 for gaseous and particulate-bound Hg(II), respectively. The nested model shows improved skill at capturing the horizontal variability of Hg observed over California during the ARCTAS aircraft campaign. The nested model suggests that North American anthropogenic emissions account for 10–22% of Hg wet deposition flux over the US, depending on the anthropogenic emissions speciation profile assumed. The modeled percent contribution can be as high as 60% near large point sources in ORV. Our results indicate that the North American anthropogenic contribution to dry deposition is 13–20%.

scholarly journals GNAQPMS-Hg v1.0, a global nested atmospheric mercury transport model: model description, evaluation and application to trans-boundary transport of Chinese anthropogenic emissions

2015 ◽  
Vol 8 (9) ◽  
pp. 2857-2876 ◽  
Author(s):  
H. S. Chen ◽  
Z. F. Wang ◽  
J. Li ◽  
X. Tang ◽  
B. Z. Ge ◽  
...  
Keyword(s):  
North America ◽  
East Asia ◽  
Aqueous Phase ◽  
Wet Deposition ◽  
Transport Model ◽  
Atmospheric Mercury ◽  
Model Description ◽  
Anthropogenic Emissions ◽  
Comparison Results ◽  
Western Asia

Abstract. Atmospheric mercury (Hg) is a toxic pollutant and can be transported over the whole globe due to its long lifetime in the atmosphere. For the purpose of assessing Hg hemispheric transport and better characterizing regional Hg pollution, a global nested atmospheric Hg transport model (GNAQPMS-Hg – Global Nested Air Quality Prediction Modeling System for Hg) has been developed. In GNAQPMS-Hg, the gas- and aqueous-phase Hg chemistry representing the transformation among three forms of Hg: elemental mercury (Hg(0)), divalent mercury (Hg(II)), and primary particulate mercury (Hg(P)) are calculated. A detailed description of the model, including mercury emissions, gas- and aqueous-phase chemistry, and dry and wet deposition is given in this study. Worldwide observations including extensive data in China have been collected for model evaluation. Comparison results show that the model reasonably simulates the global mercury budget and the spatiotemporal variation of surface mercury concentrations and deposition. Overall, model predictions of annual total gaseous mercury (TGM) and wet deposition agree with observations within a factor of 2, and within a factor of 5 for oxidized mercury and dry deposition. The model performs significantly better in North America and Europe than in East Asia. This can probably be attributed to the large uncertainties in emission inventories, coarse model resolution and to the inconsistency between the simulation and observation periods in East Asia. Compared to the global simulation, the nested simulation shows improved skill at capturing the high spatial variability of surface Hg concentrations and deposition over East Asia. In particular, the root mean square error (RMSE) of simulated Hg wet deposition over East Asia is reduced by 24 % in the nested simulation. Model sensitivity studies indicate that Chinese primary anthropogenic emissions account for 30 and 62 % of surface mercury concentrations and deposition over China, respectively. Along the rim of the western Pacific, the contributions from Chinese sources are 11 and 15.2 % over the Korean Peninsula, 10.4 and 8.2 % over Southeast Asia, and 5.7 and 5.9 % over Japan. But for North America, Europe and western Asia, the contributions from China are all below 5 %.

scholarly journals GNAQPMS-Hg v1.0, a global nested atmospheric mercury transport model: model description, evaluation and application to trans-boundary transport of Chinese anthropogenic emissions

2014 ◽  
Vol 7 (5) ◽  
pp. 6949-6996
Author(s):  
H. S. Chen ◽  
Z. F. Wang ◽  
J. Li ◽  
X. Tang ◽  
B. Z. Ge ◽  
...  
Keyword(s):  
North America ◽  
East Asia ◽  
Aqueous Phase ◽  
Wet Deposition ◽  
Transport Model ◽  
Elemental Mercury ◽  
Atmospheric Mercury ◽  
Model Description ◽  
Anthropogenic Emissions ◽  
Comparison Results

Abstract. Atmospheric mercury (Hg) is a toxic pollutant and can be transported over the whole globe due to its long lifetime in the atmosphere. For the purpose of assessing Hg hemispheric transport and better characterizing regional Hg pollution, a global nested atmospheric Hg transport model (GNAQPMS-Hg) has been developed. In GNAQPMS-Hg, the gas and aqueous phase Hg chemistry representing the transformation among three forms of Hg: elemental mercury (Hg(0)), divalent mercury (Hg(II)), and primary particulate mercury (Hg(P)) are calculated. A detailed description of the model, including mercury emissions, gas and aqueous phase chemistry, and dry and wet deposition is given in this study. Worldwide observations including extensive data in China have been collected for model evaluation. Comparison results show that the model reasonably simulates the global mercury budget and the spatial–temporal variation of surface mercury concentrations and deposition. Overall, model predictions of annual total gaseous mercury (TGM) and wet deposition agree with observations within a factor of two, and within a factor of five for oxidized mercury and dry deposition. The model performs significantly better in North America and Europe than in East Asia. This can probably be attributed to the large uncertainties in emission inventories, coarse model resolution and to the inconsistency between the simulation and observation periods in East Asia. Compared to the global simulation, the nested simulation shows improved skill at capturing the high spatial variability of Hg concentrations and deposition over East Asia. In particular, the root mean square error (RMSE) of simulated Hg wet deposition over East Asia is reduced by 24% in the nested simulation. Model sensitivity studies indicate that Chinese primary anthropogenic emissions account for 30 and 62% of surface mercury concentrations and deposition over China, respectively. Along the rim of the western Pacific, the contributions from Chinese sources are 11 and 15.2% over the Korean Peninsula, 10.4 and 8.2% over Southeast Asia, and 5.7 and 5.9% over Japan. But for North America, Europe and West Asia, the contributions from China are all below 5%.

scholarly journals Changes in dissolved iron deposition to the oceans driven by human activity: a 3-D global modelling study

2015 ◽  
Vol 12 (5) ◽  
pp. 3943-3990
Author(s):  
S. Myriokefalitakis ◽  
N. Daskalakis ◽  
N. Mihalopoulos ◽  
A. R. Baker ◽  
A. Nenes ◽  
...  
Keyword(s):  
Air Quality ◽  
Transport Model ◽  
Organic Ligand ◽  
Photochemical Reactions ◽  
Anthropogenic Emissions ◽  
Spatial And Temporal Variability ◽  
Deposition Flux ◽  
Chemical Transport Model ◽  
The Future ◽  
The Impact

Abstract. The global atmospheric iron (Fe) cycle is parameterized in the global 3-D chemical transport model TM4-ECPL to simulate the proton- and the organic ligand-promoted mineral Fe dissolution as well as the aqueous-phase photochemical reactions between the oxidative states of Fe(III/II). Primary emissions of total (TFe) and dissolved (DFe) Fe associated with dust and combustion processes are also taken into account. TFe emissions are calculated to amount to ~35 Tg Fe yr−1. The model reasonably simulates the available Fe observations, supporting the reliability of the results of this study. Accounting for proton- and organic ligand-promoted Fe-dissolution in present-day TM4-ECPL simulations, the total Fe-dissolution is calculated to be ~0.163 Tg Fe yr−1 that accounts for up to ~50% of the calculated total DFe emissions. The atmospheric burden of DFe is calculated to be ~0.012 Tg Fe. DFe deposition presents strong spatial and temporal variability with an annual deposition flux ~0.489 Tg Fe yr−1 from which about 25% (~0.124 Tg Fe yr−1) are deposited over the ocean. The impact of air-quality on Fe deposition is studied by performing sensitivity simulations using preindustrial (year 1850), present (year 2008) and future (year 2100) emission scenarios. These simulations indicate that an increase (~2 times) in Fe-dissolution may have occurred in the past 150 years due to increasing anthropogenic emissions and thus atmospheric acidity. On the opposite, a decrease (~2 times) of Fe-dissolution is projected for near future, since atmospheric acidity is expected to be lower than present-day due to air-quality regulations of anthropogenic emissions. The organic ligand contribution to Fe dissolution shows inverse relationship to the atmospheric acidity thus its importance has decreased since the preindustrial period but is projected to increase in the future. The calculated changes also show that the atmospheric DFe supply to High-Nutrient-Low-Chlorophyll oceanic areas (HNLC) characterized by Fe scarcity, has increased (~50%) since the preindustrial period. However, the DFe deposition flux is expected to decrease (~30%) to almost preindustrial levels over the Northern Hemisphere HNLC oceanic regions in the future. Significant reductions of ~20% over the Southern Ocean and the remote tropical Pacific Ocean are also projected which can further limit the primary productivity over HNLC waters.

scholarly journals Intercontinental transport and deposition patterns of atmospheric mercury from anthropogenic emissions

2014 ◽  
Vol 14 (18) ◽  
pp. 10163-10176 ◽  
Author(s):  
L. Chen ◽  
H. H. Wang ◽  
J. F. Liu ◽  
Y. D. Tong ◽  
L. B. Ou ◽  
...  
Keyword(s):  
North America ◽  
Southeast Asia ◽  
East Asia ◽  
Transport Model ◽  
Indian Subcontinent ◽  
Atmospheric Mercury ◽  
Anthropogenic Emissions ◽  
Mercury Deposition ◽  
Mercury Emissions ◽  
Source Receptor Relationships

Abstract. Global policies that regulate anthropogenic mercury emissions to the environment require quantitative and comprehensive source–receptor relationships for mercury emissions, transport and deposition among major continental regions. In this study, we use the GEOS-Chem global chemical transport model to establish source–receptor relationships among 11 major continental regions worldwide. Source–receptor relationships for surface mercury concentrations (SMC) show that some regions (e.g., East Asia, the Indian subcontinent, and Europe) should be responsible for their local surface Hg(II) and Hg(P) concentrations due to near-field transport and deposition contributions from their local anthropogenic emissions (up to 64 and 71% for Hg(II) and Hg(P), respectively, over East Asia). We define the region of primary influence (RPI) and the region of secondary influence (RSI) to establish intercontinental influence patterns. Results indicate that East Asia is the SMC RPI for almost all other regions, while Europe, Russia, and the Indian subcontinent also make some contributions to SMC over some receptor regions because they are dominant RSI source regions. Source–receptor relationships for mercury deposition show that approximately 16 and 17% of dry and wet deposition, respectively, over North America originate from East Asia, indicating that transpacific transport of East Asian emissions is the major foreign source of mercury deposition in North America. Europe, Southeast Asia, and the Indian subcontinent are also important mercury deposition sources for some receptor regions because they are the dominant RSIs. We also quantify seasonal variation on mercury deposition contributions over other regions from East Asia. Results show that mercury deposition (including dry and wet) contributions from East Asia over the Northern Hemisphere receptor regions (e.g., North America, Europe, Russia, the Middle East, and Middle Asia) vary seasonally, with the maximum values in summer and minimum values in winter. The opposite seasonal pattern occurs on mercury dry deposition contributions over Southeast Asia and the Indian subcontinent.

scholarly journals Characteristics of atmospheric mercury deposition and size-fractionated particulate mercury in urban Nanjing, China

2014 ◽  
Vol 14 (5) ◽  
pp. 2233-2244 ◽  
Author(s):  
J. Zhu ◽  
T. Wang ◽  
R. Talbot ◽  
H. Mao ◽  
X. Yang ◽  
...  
Keyword(s):  
Dry Deposition ◽  
Wet Deposition ◽  
Fine Particles ◽  
Unit Area ◽  
Atmospheric Mercury ◽  
Anthropogenic Sources ◽  
Deposition Flux ◽  
Coarse Particles ◽  
Mercury Deposition ◽  
Particulate Mercury

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.

scholarly journals Overview of mercury dry deposition, litterfall, and throughfall studies

2016 ◽  
Author(s):  
L. Paige Wright ◽  
Leiming Zhang ◽  
Frank J. Marsik
Keyword(s):  
North America ◽  
Dry Deposition ◽  
Wet Deposition ◽  
Current Knowledge ◽  
Measurement Methods ◽  
Anthropogenic Emissions ◽  
Transport Models ◽  
Modelling Method ◽  
Chemical Transport Models ◽  
Or Modelling

Abstract. The current knowledge concerning mercury dry deposition is reviewed, including dry deposition algorithms used in chemical transport models (CTMs) and at monitoring sites and related deposition calculations, measurement methods and studies for quantifying dry deposition of gaseous oxidized mercury (GOM) and particulate bound mercury (PBM), and measurement studies of litterfall and throughfall mercury. Measured median GOM plus PBM dry deposition in Asia (10.7 μg m−2 yr−1) almost double that in North America (6.1 μg m−2 yr−1) due to the higher anthropogenic emissions in Asia. Measured median litterfall and throughfall mercury are 22.3 and 56.5 μg m−2 yr−1, respectively, in Asia, 12.8 and 16.3 μg m−2 yr−1 in Europe, and 11.9 and 7.0 μg m−2 yr−1 in North America. The much higher litterfall mercury than GOM plus PBM dry deposition suggests the important contribution of gaseous elemental mercy (GEM) to mercury dry deposition to vegetated canopies. Over all the regions, including the Amazon, dry deposition, estimated as the sum of litterfall and throughfall minus open-field wet deposition, is more dominant than wet deposition for Hg deposition. Regardless of the measurement or modelling method used, a factor of two or larger uncertainties in GOM plus PBM dry deposition need to be kept in mind when using these numbers for mercury impact studies.

scholarly journals Impacts of Anthropogenic Emissions and Meteorological Variation on Hg Wet Deposition in Chongming, China

Atmosphere ◽  
2020 ◽  
Vol 11 (12) ◽  
pp. 1301
Author(s):  
Yi Tang ◽  
Qingru Wu ◽  
Wei Gao ◽  
Shuxiao Wang ◽  
Zhijian Li ◽  
...  
Keyword(s):  
Wet Deposition ◽  
Warm Season ◽  
Meteorological Condition ◽  
Anthropogenic Emissions ◽  
Deposition Flux ◽  
Wet Deposition Flux ◽  
Meteorological Variation ◽  
Global Concern ◽  
The Impact

Mercury (Hg) is a ubiquitous environmental toxicant that has caused global concern due to its persistence and bioaccumulation in the environment. Wet deposition is a crucial Hg input for both terrestrial and aquatic environments and is a significant indicator for evaluating the effectiveness of anthropogenic Hg control. Rainwater samples were collected from May 2014 to October 2018 in Chongming Island to understand the multi-year Hg wet deposition characteristics. The annual Hg wet deposition flux ranged from 2.6 to 9.8 μg m−2 yr−1 (mean: 4.9 μg m−2 yr−1). Hg wet deposition flux in Chongming was comparable to the observations at temperate and subtropical background sites (2.0–10.2 μg m−2 yr−1) in the northern hemisphere. Hg wet deposition flux decreased from 8.6 μg m−2 yr−1 in 2014–2015 to 3.8 μg m−2 yr−1 in 2016 and was attributed to a decrease in the volume-weighted mean (VWM) Hg concentration (−4.1 ng L−1 yr−1). The reduced VWM Hg was explained by the decreasing atmospheric Hg and anthropogenic emissions reductions. The annual Hg wet deposition flux further decreased from 3.8 μg m−2 in 2016 to 2.6 μg m−2 in 2018. The reduction of warm season (April–September) rainfall amounts (356–845 mm) mainly contributed to the Hg wet deposition flux reduction during 2016–2018. The multi-year monitoring results suggest that long-term measurements are necessary when using wet deposition as an indicator to reflect the impact of anthropogenic efforts on mercury pollution control and meteorological condition variations.

scholarly journals Bioavailable atmospheric phosphorous supply to the global ocean: a 3-D global modeling study

2016 ◽  
Vol 13 (24) ◽  
pp. 6519-6543 ◽  
Author(s):  
Stelios Myriokefalitakis ◽  
Athanasios Nenes ◽  
Alex R. Baker ◽  
Nikolaos Mihalopoulos ◽  
Maria Kanakidou
Keyword(s):  
Transport Model ◽  
Mineral Dust ◽  
Current Knowledge ◽  
Marine Ecosystem ◽  
Anthropogenic Sources ◽  
Global Ocean ◽  
Spatial And Temporal Variability ◽  
Deposition Flux ◽  
P Solubilization ◽  
Global Study

Abstract. The atmospheric cycle of phosphorus (P) is parameterized here in a state-of-the-art global 3-D chemistry transport model, taking into account primary emissions of total P (TP) and soluble P (DP) associated with mineral dust, combustion particles from natural and anthropogenic sources, bioaerosols, sea spray and volcanic aerosols. For the present day, global TP emissions are calculated to be roughly 1.33 Tg-P yr−1, with the mineral sources contributing more than 80 % to these emissions. The P solubilization from mineral dust under acidic atmospheric conditions is also parameterized in the model and is calculated to contribute about one-third (0.14 Tg-P yr−1) of the global DP atmospheric source. To our knowledge, a unique aspect of our global study is the explicit modeling of the evolution of phosphorus speciation in the atmosphere. The simulated present-day global annual DP deposition flux is 0.45 Tg-P yr−1 (about 40 % over oceans), showing a strong spatial and temporal variability. Present-day simulations of atmospheric P aerosol concentrations and deposition fluxes are satisfactory compared with available observations, indicating however an underestimate of about 70 % on current knowledge of the sources that drive the P atmospheric cycle. Sensitivity simulations using preindustrial (year 1850) anthropogenic and biomass burning emission scenarios showed a present-day increase of 75 % in the P solubilization flux from mineral dust, i.e., the rate at which P is converted into soluble forms, compared to preindustrial times, due to increasing atmospheric acidity over the last 150 years. Future reductions in air pollutants due to the implementation of air-quality regulations are expected to decrease the P solubilization flux from mineral dust by about 30 % in the year 2100 compared to the present day. Considering, however, that all the P contained in bioaerosols is readily available for uptake by marine organisms, and also accounting for all other DP sources, a total bioavailable P flux of about 0.17 Tg-P yr−1 to the oceans is derived. Our calculations further show that in some regions more than half of the bioavailable P deposition flux to the ocean can originate from biological particles, while this contribution is found to maximize in summer when atmospheric deposition impact on the marine ecosystem is the highest due to ocean stratification. Thus, according to this global study, a largely unknown but potentially important role of terrestrial bioaerosols as suppliers of bioavailable P to the global ocean is also revealed. Overall, this work provides new insights to the atmospheric P cycle by demonstrating that biological materials are important carriers of bioavailable P, with very important implications for past and future responses of marine ecosystems to global change.

scholarly journals Subtropical subsidence and surface deposition of oxidized mercury produced in the free troposphere

2017 ◽  
Vol 17 (14) ◽  
pp. 8999-9017 ◽  
Author(s):  
Viral Shah ◽  
Lyatt Jaeglé
Keyword(s):  
Boundary Layer ◽  
Dry Deposition ◽  
Wet Deposition ◽  
Transport Model ◽  
Lower Troposphere ◽  
Deposition Flux ◽  
Surface Deposition ◽  
Middle Troposphere ◽  
Western Us ◽  
Wet Deposition Flux

Abstract. Oxidized mercury (Hg(II)) is chemically produced in the atmosphere by oxidation of elemental mercury and is directly emitted by anthropogenic activities. We use the GEOS-Chem global chemical transport model with gaseous oxidation driven by Br atoms to quantify how surface deposition of Hg(II) is influenced by Hg(II) production at different atmospheric heights. We tag Hg(II) chemically produced in the lower (surface–750 hPa), middle (750–400 hPa), and upper troposphere (400 hPa–tropopause), in the stratosphere, as well as directly emitted Hg(II). We evaluate our 2-year simulation (2013–2014) against observations of Hg(II) wet deposition as well as surface and free-tropospheric observations of Hg(II), finding reasonable agreement. We find that Hg(II) produced in the upper and middle troposphere constitutes 91 % of the tropospheric mass of Hg(II) and 91 % of the annual Hg(II) wet deposition flux. This large global influence from the upper and middle troposphere is the result of strong chemical production coupled with a long lifetime of Hg(II) in these regions. Annually, 77–84 % of surface-level Hg(II) over the western US, South America, South Africa, and Australia is produced in the upper and middle troposphere, whereas 26–66 % of surface Hg(II) over the eastern US, Europe, and East Asia, and South Asia is directly emitted. The influence of directly emitted Hg(II) near emission sources is likely higher but cannot be quantified by our coarse-resolution global model (2° latitude  ×  2.5° longitude). Over the oceans, 72 % of surface Hg(II) is produced in the lower troposphere because of higher Br concentrations in the marine boundary layer. The global contribution of the upper and middle troposphere to the Hg(II) dry deposition flux is 52 %. It is lower compared to the contribution to wet deposition because dry deposition of Hg(II) produced aloft requires its entrainment into the boundary layer, while rain can scavenge Hg(II) from higher altitudes more readily. We find that 55 % of the spatial variation of Hg wet deposition flux observed at the Mercury Deposition Network sites is explained by the combined variation of precipitation and Hg(II) produced in the upper and middle troposphere. Our simulation points to a large role of the dry subtropical subsidence regions. Hg(II) present in these regions accounts for 74 % of Hg(II) at 500 hPa over the continental US and more than 60 % of the surface Hg(II) over high-altitude areas of the western US. Globally, it accounts for 78 % of the tropospheric Hg(II) mass and 61 % of the total Hg(II) deposition. During the Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) aircraft campaign, the contribution of Hg(II) from the dry subtropical regions was found to be 75 % when measured Hg(II) exceeded 250 pg m−3. Hg(II) produced in the upper and middle troposphere subsides in the anticyclones, where the dry conditions inhibit the loss of Hg(II). Our results highlight the importance the subtropical anticyclones as the primary conduits for the production and export of Hg(II) to the global atmosphere.

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