scholarly journals Relative contributions of gaseous oxidized mercury and fine and coarse particle‐bound mercury to mercury wet deposition at nine monitoring sites in North America

2015 ◽  
Vol 120 (16) ◽  
pp. 8549-8562 ◽  
Author(s):  
Irene Cheng ◽  
Leiming Zhang ◽  
Huiting Mao
Keyword(s):  
North America ◽  
Wet Deposition ◽  
Coarse Particle ◽  
Gaseous Oxidized Mercury

scholarly journals Multi-model study of HTAP II on sulphur and nitrogen deposition

2018 ◽  
Author(s):  
Jiani Tan ◽  
Joshua S. Fu ◽  
Frank Dentener ◽  
Jian Sun ◽  
Louisa Emmons ◽  
...  
Keyword(s):  
North America ◽  
East Asia ◽  
South Asia ◽  
Wet Deposition ◽  
Task Force ◽  
East Asian ◽  
Control Policy ◽  
N Deposition ◽  
Eastern United States ◽  
S Deposition

Abstract. This study uses multi-model ensemble results of 11 models from the 2nd phase of Task Force Hemispheric Transport of Air Pollution (HTAP II) to calculate the global sulfur (S) and nitrogen (N) deposition in 2010. Modelled wet deposition is evaluated with observation networks in North America, Europe and Asia. The modelled results agree well with observations, with 76–83 % of stations having predicted within ±50 % of observations. The results underestimate SO42−, NO3− and NH4+ wet depositions in some European and East Asian stations, but overestimate NO3− wet deposition in Eastern United States. Inter-comparison with previous projects (PhotoComp, ACCMIP and HTAP I) shows HTPA II has considerably improved the estimation of deposition at European and East Asian stations. Modelled dry deposition is generally higher than the “inferential” data calculated by observed concentration and modelled velocity in North America, but the inferential data has high uncertainty, too. The global S deposition is 84 Tg(S) in 2010, with 49 % of the deposits on continental regions and 51 % on ocean (19 % on coastal). The global N deposition consists of 59 Tg(N) oxidized nitrogen (NOy) deposition and 64 Tg(N) reduced nitrogen (NHx) deposition in 2010. 65 % of N is deposited on the continental regions and 35 % is on ocean (15 % on coastal). The estimated outflow of pollution from land to ocean is about 4 Tg(S) for S deposition and 18 Tg(N) for N deposition. Compared our results to the results in 2001 from HTAP I, we find that the global distributions of S and N depositions have changed considerably during the last 10 years. The global S deposition decreases 2 Tg(S) (3 %) from 2001 to 2010, with significant decreases in Europe (5 Tg(S) and 55 %), North America (3 Tg(S) and 29 %) and Russia (2 Tg(S) and 26 %), and increases in South Asia (2 Tg(S) and 42 %) and the Middle East (1 Tg(S) and 44% ). The global N deposition increases by 7 Tg(N) (6 %), mainly contributed by South Asia (5 Tg(N) and 39 %), East Asia (4 Tg(N) and 21 %) and Southeast Asia (2 Tg(N) and 21 %). The NHx deposition is increased with no control policy on NH3 emission in North America. On the other hand, NOy deposition starts to dominate in East Asia (especially China) due to boosted NOx emission in recent years.

scholarly journals Evaluation of global EMEP MSC-W (rv4.34) WRF (v3.9.1.1) model surface concentrations and wet deposition of reactive N and S with measurements

2021 ◽  
Vol 14 (11) ◽  
pp. 7021-7046
Author(s):  
Yao Ge ◽  
Mathew R. Heal ◽  
David S. Stevenson ◽  
Peter Wind ◽  
Massimo Vieno
Keyword(s):  
North America ◽  
Southeast Asia ◽  
East Asia ◽  
Atmospheric Chemistry ◽  
Wet Deposition ◽  
Global Analysis ◽  
Monitoring Networks ◽  
Model Framework ◽  
Annual Total ◽  
Model Measurement

Abstract. Atmospheric pollution has many profound effects on human health, ecosystems, and the climate. Of concern are high concentrations and deposition of reactive nitrogen (Nr) species, especially of reduced N (gaseous NH3, particulate NH4+). Atmospheric chemistry and transport models (ACTMs) are crucial to understanding sources and impacts of Nr chemistry and its potential mitigation. Here we undertake the first evaluation of the global version of the EMEP MSC-W ACTM driven by WRF meteorology (1∘×1∘ resolution), with a focus on surface concentrations and wet deposition of N and S species relevant to investigation of atmospheric Nr and secondary inorganic aerosol (SIA). The model–measurement comparison is conducted both spatially and temporally, covering 10 monitoring networks worldwide. Model simulations for 2010 compared use of both HTAP and ECLIPSEE (ECLIPSE annual total with EDGAR monthly profile) emissions inventories; those for 2015 used ECLIPSEE only. Simulations of primary pollutants are somewhat sensitive to the choice of inventory in places where regional differences in primary emissions between the two inventories are apparent (e.g. China) but are much less sensitive for secondary components. For example, the difference in modelled global annual mean surface NH3 concentration using the two 2010 inventories is 18 % (HTAP: 0.26 µg m−3; ECLIPSEE: 0.31 µg m−3) but is only 3.5 % for NH4+ (HTAP: 0.316 µg m−3; ECLIPSEE: 0.305 µg m−3). Comparisons of 2010 and 2015 surface concentrations between the model and measurements demonstrate that the model captures the overall spatial and seasonal variations well for the major inorganic pollutants NH3, NO2, SO2, HNO3, NH4+, NO3-, and SO42- and their wet deposition in East Asia, Southeast Asia, Europe, and North America. The model shows better correlations with annual average measurements for networks in Southeast Asia (mean R for seven species: R7‾=0.73), Europe (R7‾=0.67), and North America (R7‾=0.63) than in East Asia (R5‾=0.35) (data for 2015), which suggests potential issues with the measurements in the latter network. Temporally, both model and measurements agree on higher NH3 concentrations in spring and summer and lower concentrations in winter. The model slightly underestimates annual total precipitation measurements (by 13 %–45 %) but agrees well with the spatial variations in precipitation in all four world regions (0.65–0.94 R range). High correlations between measured and modelled NH4+ precipitation concentrations are also observed in all regions except East Asia. For annual total wet deposition of reduced N, the greatest consistency is in North America (0.75–0.82 R range), followed by Southeast Asia (R=0.68) and Europe (R=0.61). Model–measurement bias varies between species in different networks; for example, bias for NH4+ and NO3- is largest in Europe and North America and smallest in East Asia and Southeast Asia. The greater uniformity in spatial correlations than in biases suggests that the major driver of model–measurement discrepancies (aside from differing spatial representativeness and uncertainties and biases in measurements) are shortcomings in absolute emissions rather than in modelling the atmospheric processes. The comprehensive evaluations presented in this study support the application of this model framework for global analysis of current and potential future budgets and deposition of Nr and SIA.

scholarly journals Update on emissions and environmental impacts from the international fleet of ships. The contribution from major ship types and ports

2008 ◽  
Vol 8 (5) ◽  
pp. 18323-18384 ◽  
Author(s):  
S. B. Dalsøren ◽  
M. S. Eide ◽  
Ø. Endresen ◽  
A. Mjelde ◽  
G. Gravir ◽  
...  
Keyword(s):  
North America ◽  
Wet Deposition ◽  
Western Europe ◽  
Surface Ozone ◽  
Western North America ◽  
Ship Emissions ◽  
Low Latitudes ◽  
The World ◽  
Emission Modelling ◽  
The Impact

Abstract. A reliable and up-to-date ship emission inventory is essential for atmospheric scientists quantifying the impact of shipping and for policy makers implementing regulations and incentives for emission reduction. The emission modelling in this study takes into account ship type and size dependent input data for 15 ship types and 7 size categories. Global port arrival and departure data for more than 32 000 merchant ships are used to establish operational profiles for the ship segments. The modelled total fuel consumption amounts to 217 Mt in 2004 of which 11 Mt is consumed in in-port operations. This is in agreement with international sales statistics. The modelled fuel consumption is applied to develop global emission inventories for CO2, NO2, SO2, CO, CH4, VOC (Volatile Organic Compounds), N2O, BC (Black Carbon) and OC (Organic Carbon). The global emissions from ships at sea and in ports are distributed geographically, applying extended geographical data sets covering about 2 million global ship observations and global port data for 32 000 ships. In addition to inventories for the world fleet, inventories are produced separately for the three dominating ship types, using ship type specific emission modelling and traffic distributions. A global Chemical Transport Model (CTM) was used to calculate the environmental impacts of the emissions. We find that ship emissions is a dominant contributor over much of the world oceans to surface concentrations of NO2 and SO2. The contribution is also large over some coastal zones. For surface ozone the contribution is high over the oceans but clearly also of importance over western North America (contribution 15–25%) and western Europe (5–15%). The contribution to tropospheric column ozone is up to 5–6%. The overall impact of ship emissions on global methane lifetime is large due to the high NOx emissions. With regard to acidification we find that ships contribute 11% to nitrate wet deposition and 4.5% to sulphur wet deposition globally. In certain coastal regions the contributions may be in the range 15–50%. In general we find that ship emissions have a large impact on acidic deposition and surface ozone in western North America, Scandinavia, western Europe, western North Africa and Malaysia/Indonesia. For most of these regions container traffic, the largest emitter by ship type, has the largest impact. This is the case especially for the Pacific and the related container trade routes between Asia and North America. However, the contributions from bulk ships and tank vessels are also significant in the above mentioned impact regions. Though the total ship impact at low latitudes is lower, the tank vessels have a quite large contribution at low latitudes and near the Gulf of Mexico and Middle East. The bulk ships are characterized by large impact in Oceania compared to other ship types. In Scandinavia and north-western Europe, one of the major ship impact regions, the three largest ship types have rather small relative contributions. The impact in this region is probably dominated by smaller ships operating closer to the coast. For emissions in ports impacts on NO2 and SO2 seem to be of significance. For most ports the contribution to the two components is in the range 0.5–5%, for a few ports it exceeds 10%. The approach presented provides an improvement in characterizing fleet operational patterns, and thereby ship emissions and impacts. Furthermore, the study shows where emission reductions can be applied to most effectively minimize the impacts by different ship types.

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 Update on emissions and environmental impacts from the international fleet of ships: the contribution from major ship types and ports

2009 ◽  
Vol 9 (6) ◽  
pp. 2171-2194 ◽  
Author(s):  
S. B. Dalsøren ◽  
M. S. Eide ◽  
Ø. Endresen ◽  
A. Mjelde ◽  
G. Gravir ◽  
...  
Keyword(s):  
North America ◽  
Wet Deposition ◽  
Western Europe ◽  
Surface Ozone ◽  
Western North America ◽  
Ship Emissions ◽  
Low Latitudes ◽  
The World ◽  
Emission Modelling ◽  
The Impact

Abstract. A reliable and up-to-date ship emission inventory is essential for atmospheric scientists quantifying the impact of shipping and for policy makers implementing regulations and incentives for emission reduction. The emission modelling in this study takes into account ship type and size dependent input data for 15 ship types and 7 size categories. Global port arrival and departure data for more than 32 000 merchant ships are used to establish operational profiles for the ship segments. The modelled total fuel consumption amounts to 217 Mt in 2004 of which 11 Mt is consumed in in-port operations. This is in agreement with international sales statistics. The modelled fuel consumption is applied to develop global emission inventories for CO2, NO2, SO2, CO, CH4, VOC (Volatile Organic Compounds), N2O, BC (Black Carbon) and OC (Organic Carbon). The global emissions from ships at sea and in ports are distributed geographically, applying extended geographical data sets covering about 2 million global ship observations and global port data for 32 000 ships. In addition to inventories for the world fleet, inventories are produced separately for the three dominating ship types, using ship type specific emission modelling and traffic distributions. A global Chemical Transport Model (CTM) was used to calculate the environmental impacts of the emissions. We find that ship emissions is a dominant contributor over much of the world oceans to surface concentrations of NO2 and SO2. The contribution is also large over some coastal zones. For surface ozone the contribution is high over the oceans but clearly also of importance over Western North America (contribution 15–25%) and Western Europe (5–15%). The contribution to tropospheric column ozone is up to 5–6%. The overall impact of ship emissions on global methane lifetime is large due to the high NOx emissions. With regard to acidification we find that ships contribute 11% to nitrate wet deposition and 4.5% to sulphur wet deposition globally. In certain coastal regions the contributions may be in the range 15–50%. In general we find that ship emissions have a large impact on acidic deposition and surface ozone in Western North America, Scandinavia, Western Europe, western North Africa and Malaysia/Indonesia. For most of these regions container traffic, the largest emitter by ship type, has the largest impact. This is the case especially for the Pacific and the related container trade routes between Asia and North America. However, the contributions from bulk ships and tank vessels are also significant in the above mentioned impact regions. Though the total ship impact at low latitudes is lower, the tank vessels have a quite large contribution at low latitudes and near the Gulf of Mexico and Middle East. The bulk ships are characterized by large impact in Oceania compared to other ship types. In Scandinavia and north-Western Europe, one of the major ship impact regions, the three largest ship types have rather small relative contributions. The impact in this region is probably dominated by smaller ships operating closer to the coast. For emissions in ports impacts on NO2 and SO2 seem to be of significance. For most ports the contribution to the two components is in the range 0.5–5%, for a few ports it exceeds 10%. The approach presented provides an improvement in characterizing fleet operational patterns, and thereby ship emissions and impacts. Furthermore, the study shows where emission reductions can be applied to most effectively minimize the impacts by different ship types.

Aggregation of Selected Three-Day Periods to Estimate Annual and Seasonal Wet Deposition Totals for Sulfate, Nitrate, and Acidity. Part I: A Synoptic and Chemical Climatology for Eastern North America

1995 ◽  
Vol 34 (2) ◽  
pp. 297-325 ◽  
Author(s):  
Jeffrey R. Brook ◽  
Perry J. Samson ◽  
Sanford Sillman
Keyword(s):  
North America ◽  
Wet Deposition ◽  
Atmospheric Transport ◽  
Precipitation Amount ◽  
Statistical Correlation ◽  
Eastern North America ◽  
Time Of Year ◽  
Transport Patterns

Abstract Running 3-day periods from 1979 to 1985 were categorised into one of 20 meteorological categories. These categories were developed through the cluster analysis of 3-day progressions of 85-kPa wind flow over eastern North America. The purpose for developing the categories was to identify recurring atmospheric transport patterns that were associated with differing amounts of wet sulfate (SO2−4) and nitrate (NO−3) deposition at a variety of locations in eastern North America. Identification of these patterns was necessary to facilitate the selection of time periods for simulation by the Regional Acid Deposition Model and in the development of a method for estimating long-term acidic deposition over eastern North America from a limited number of model runs. The effectiveness of this method (referred to as the aggregation method) was expected to be dependent on the ability of the categories to separate structure in wet deposition patterns. This paper describes the determination of the 20 meteorological categories and demonstrates that there were differences in their meteorological and chemical behavior and in their frequency of occurrence. Observations of precipitation and wet SO2−4 and NO−3 deposition from 22 sites in eastern North America and multiple regression models were used to demonstrate that there were statistically significant differences in deposition among categories and that knowledge of meteorological category explained some of the variation in wet deposition. The best statistical correlation, which was based upon precipitation amount, time of year, and meteorological category, explained 35%–83% (28%– 76%) of the observed variation in wet SO2−4 (NO−3) deposition depending on location. On average, across all sites and for both SO2−4 and NO−3, knowledge of category accounted for about 4% of the variation. The minimum amount explained by category was 1% and the maximum was 13%.

scholarly journals Evaluation of global EMEP MSC-W (rv4.34)-WRF (v3.9.1.1) model surface concentrations and wet deposition of reactive N and S with measurements

2021 ◽  
Author(s):  
Yao Ge ◽  
Mathew R. Heal ◽  
David S. Stevenson ◽  
Peter Wind ◽  
Massimo Vieno
Keyword(s):  
North America ◽  
Southeast Asia ◽  
East Asia ◽  
Atmospheric Chemistry ◽  
Wet Deposition ◽  
Global Analysis ◽  
Monitoring Networks ◽  
Model Framework ◽  
Annual Total ◽  
Model Measurement

Abstract. Atmospheric pollution has many profound effects on human health, ecosystems, and the climate. Of concern are high concentrations and deposition of reactive nitrogen (Nr) species, especially of reduced N (gaseous NH3, particulate NH4+). Atmospheric chemistry and transport models (ACTMs) are crucial to understanding sources and impacts of Nr chemistry and its potential mitigation. Here we undertake the first evaluation of the global version of the EMEP MSC-W ACTM driven by WRF meteorology (1° × 1° resolution), with a focus on surface concentrations and wet deposition of N and S species relevant to investigation of atmospheric Nr and secondary inorganic aerosol (SIA). The model-measurement comparison is conducted both spatially and temporally, covering 9 monitoring networks worldwide. Model simulations for 2010 compared use of both HTAP and ECLIPSEE (ECLIPSE annual total with EDGAR monthly profile) emissions inventories; those for 2015 used ECLIPSEE only. Simulations of primary pollutants are somewhat sensitive to the choice of inventory in places where regional differences in primary emissions between the two inventories are apparent (e.g. China), but much less so for secondary components. For example, the difference in modelled global annual mean surface NH3 concentration using the two 2010 inventories is 18 % (HTAP: 0.26 μg m−3; ECLIPSEE: 0.31 μg m−3) but only 3.5 % for NH4+ (HTAP: 0.316 μg m−3; ECLIPSEE: 0.305 μg m−3). Comparisons of 2010 and 2015 surface concentrations between model and measurement demonstrate that the model captures well the overall spatial and seasonal variations of the major inorganic pollutants NH3, NO2, SO2, HNO3, NH4+, NO3−, SO42−, and their wet deposition in East Asia, Southeast Asia, Europe and North America. The model shows better correlations with annual average measurements for networks in Southeast Asia (Mean R for 7 species:  = 0.73), Europe ( = 0.67) and North America ( = 0.63) than in East Asia ( = 0.35) (data for 2015), which suggests potential issues with the measurements in the latter network. Temporally, both model and measurement agree on higher NH3 concentrations in spring and summer, and lower concentrations in winter. The model slightly underestimates annual total precipitation measurements (by 13–34 %) but agrees well with the spatial variations in precipitation in all four world regions (0.65–0.78 R range). High correlations between measured and modelled NH4+ precipitation concentrations are also observed in all regions except East Asia. For annual total wet deposition of reduced N, the greatest consistency is in North America (R = 0.75), followed by Southeast Asia (R = 0.68) and Europe (R = 0.61). Model-measurement bias varies between species in different networks; for example, bias for NH4+ and NO3− is most in Europe and North America and least in East and Southeast Asia. The greater uniformity in spatial correlations than in biases suggests that the major driver of model-measurement discrepancies (aside from differing spatial representativeness and uncertainties and biases in measurements) are shortcomings in absolute emissions rather than in modelling the atmospheric processes. The comprehensive evaluations presented in this study support the application of this model framework for global analysis of current and potential future budgets and deposition of Nr and SIA.

scholarly journals Evaluation of discrepancy between measured and modeled oxidized mercury species

2012 ◽  
Vol 12 (7) ◽  
pp. 17245-17293 ◽  
Author(s):  
G. Kos ◽  
A. Ryzhkov ◽  
A. Dastoor ◽  
J. Narayan ◽  
A. Steffen ◽  
...  
Keyword(s):  
North America ◽  
Wet Deposition ◽  
Regional Scale ◽  
Anthropogenic Sources ◽  
Mercury Species ◽  
Emission Sources ◽  
Eastern United States ◽  
Measured Concentration ◽  
Yearly Average ◽  
High Emission

Abstract. Zhang et al. (2012a), in a recent report, compared model estimates and new observations of oxidised and particulate mercury species (Hg2+ and Hgp) in the Great Lakes region and found that the sum of Hg2+ and Hgp varied between a factor of 2 to 10 between measurements and model. They suggested too high emission inputs and too fast oxidative conversion of Hg0 to Hg2+ and Hgp, as possible causes. This study quantitatively explores in detail the uncertainties in measurements, in addition to the above concerns and speciation of mercury near emission sources in the model to better understand these discrepancies in the context of oxidized mercury, i.e. gaseous (Hg2+) and particulate (Hgp) mercury. These include sampling efficiency, composition of sample, interfering species and calibration errors for measurements and in-plume reduction processes. Sensitivity simulations using Global/Regional Atmospheric Heavy Metals Model (GRAHM) were performed to analyze the role of in-plume reduction on ambient concentrations and deposition of mercury in North America. The discrepancy between simulated and observed concentrations of Hg2+ and Hgp was found to be reduced when a ratio for Hg0:Hg2+:Hgp in the emissions was changed from 50:40:10 (as specified in the original inventories) to 90:8:2 to account for in-plume reduction of Hg0 processes. A significant reduction of the root mean square error (e.g., 19.22 to 11.3 pg m−3 for New Jersey site NJ54) and bias (67.8 to 19.3 pg m−3 for NJ54) for sampling sites in the Eastern United States and Canada, especially for sites near emission sources was found. Significant improvements in the spatial distribution of wet deposition of mercury in North America was noticed. Particularly, over-prediction of wet deposition near anthropogenic sources of mercury was reduced by 43%. On a regional scale, estimated wet deposition improved by a factor of 2 for areas with more than 12 μg m−2 yearly average wet deposition. Model sensitivity simulations show that the measured concentration of oxidized mercury is too low to be consistent with measured wet deposition fluxes in North America. This improvement by a factor of 2 and measurement uncertainties within a factor of 3 to 8 provides a reasonable rationale for the discrepancy of a factor of 2–10 determined by Zhang et al. (2012a).

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