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 ◽  
...  

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.

2013 ◽  
Vol 13 (9) ◽  
pp. 25185-25218 ◽  
Author(s):  
L. Chen ◽  
H.-H. Wang ◽  
J.-F. Liu ◽  
W. Zhang ◽  
D. Hu ◽  
...  

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 model to establish source–receptor relationships among eleven 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 because of 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 region of primary influence (RPI) and region of secondary influence (RSI) to establish intercontinental influence patterns. Results indicate that East Asia is 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 trans-pacific 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 dominant RSI. 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, 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.


2015 ◽  
Vol 8 (9) ◽  
pp. 2857-2876 ◽  
Author(s):  
H. S. Chen ◽  
Z. F. Wang ◽  
J. Li ◽  
X. Tang ◽  
B. Z. Ge ◽  
...  

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 %.


2014 ◽  
Vol 7 (5) ◽  
pp. 6949-6996
Author(s):  
H. S. Chen ◽  
Z. F. Wang ◽  
J. Li ◽  
X. Tang ◽  
B. Z. Ge ◽  
...  

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%.


2009 ◽  
Vol 9 (5) ◽  
pp. 21285-21315
Author(s):  
C.-J. Lin ◽  
L. Pan ◽  
D. G. Streets ◽  
S. K. Shetty ◽  
C. Jang ◽  
...  

Abstract. East Asia contributes nearly 50% of the global anthropogenic mercury emissions into the atmosphere. Recently, there are concerns for the long-range transport of mercury from East Asia to North America, which may lead to enhanced dry and wet depositions in North America. In this study, we performed four monthly simulations (January, April, July and October in 2005) using CMAQ-Hg v4.6 in an East Asian model domain. Coupled with a mass balance analysis and a number of emission inventory scenarios, the chemical transport of atmospheric mercury, the seasonal mercury transport budgets and mercury emission outflow from the East Asian region were investigated. The total annual mercury deposition in the region for the modeling year is estimated to be 821 Mg, with 396 Mg contributed by wet deposition and 425 Mg contributed by dry deposition. Regional mercury transport budgets show strong seasonal variability, with a net removal of RGM (7~5 Mg mo−1) and PHg (13~21 Mg mo−1), and a net export of GEM (60~130 Mg mo−1) from the study domain. The annual outflow caused by the East Asian emission is estimated to be in the range of 1369~1671 Mg yr−1, primarily in the form of GEM. This represents about 75% of the total mercury emissions (anthropogenic and natural) in the region. The emission outflow from this source region would contribute to 20~30% of mercury deposition in areas remote from anthropogenic emission sources.


2012 ◽  
Vol 12 (1) ◽  
pp. 2603-2646 ◽  
Author(s):  
Y. Zhang ◽  
L. Jaeglé ◽  
A. van Donkelaar ◽  
R. V. Martin ◽  
C. D. Holmes ◽  
...  

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%.


2010 ◽  
Vol 7 (6) ◽  
pp. 537 ◽  
Author(s):  
Anne L. Soerensen ◽  
Henrik Skov ◽  
Matthew S. Johnson ◽  
Marianne Glasius

Environmental context Mercury is a neurotoxin that bioaccumulates in the aquatic food web. Atmospheric emissions from urban areas close to the coast could cause increased local mercury deposition to the ocean. Our study adds important new data to the current limited knowledge on atmospheric mercury emissions and dynamics in coastal urban areas. Abstract Approximately 50% of primary atmospheric mercury emissions are anthropogenic, resulting from e.g. emission hotspots in urban areas. Emissions from urban areas close to the coast are of interest because they could increase deposition loads to nearby coastal waters as well as contribute to long range transport of mercury. We present results from measurements of gaseous elemental mercury (GEM) and reactive gaseous mercury (RGM) in 15 coastal cities and their surrounding marine boundary layer (MBL). An increase of 15–90% in GEM concentration in coastal urban areas was observed compared with the remote MBL. Strong RGM enhancements were only found in two cities. In urban areas with statistically significant GEM/CO enhancement ratios, slopes between 0.0020 and 0.0087 ng m–3 ppb–1 were observed, which is consistent with other observations of anthropogenic enhancement. The emission ratios were used to estimate GEM emissions from the areas. A closer examination of data from Sydney (Australia), the coast of Chile, and Valparaiso region (Chile) in the southern hemisphere, is presented.


2018 ◽  
Author(s):  
Arlene M. Fiore ◽  
Emily V. Fischer ◽  
Shubha Pandey Deolal ◽  
Oliver Wild ◽  
Dan Jaffe ◽  
...  

Abstract. Peroxy acetyl nitrate (PAN) is the most important reservoir species for nitrogen oxides (NOx) in the remote troposphere. Upon decomposition in remote regions, PAN promotes efficient ozone production. We evaluate monthly mean PAN abundances from global chemical transport model simulations (HTAP1) for 2001 with measurements from five northern mid-latitude mountain sites (four European and one North American). The multi-model mean generally captures the observed monthly mean PAN but individual models simulate a factor of ~ 4–8 range in monthly abundances. We quantify PAN source-receptor relationships at the measurement sites with sensitivity simulations that decrease regional anthropogenic emissions of PAN (and ozone) precursors by 20 % from North America (NA), Europe (EU), and East Asia (EA). The HTAP1 models attribute more of the observed PAN at Jungfraujoch (Switzerland) to emissions in NA and EA, and less to EU, than a prior trajectory-based estimate. The trajectory-based and modeling approaches agree that EU emissions play a role in the observed springtime PAN maximum at Jungfraujoch. The signal from anthropogenic emissions on PAN is strongest at Jungfraujoch and Mount Bachelor (Oregon, U.S.A.) during April. In this month, PAN source-receptor relationships correlate both with model differences in regional anthropogenic volatile organic compound (AVOC) emissions and with ozone source-receptor relationships. PAN observations at mountaintop sites can thus provide key information for evaluating models, including links between PAN and ozone production and source-receptor relationships. Establishing routine, long-term, mountaintop measurements is essential given the large observed interannual variability in PAN.


2021 ◽  
Vol 14 (11) ◽  
pp. 7021-7046
Author(s):  
Yao Ge ◽  
Mathew R. Heal ◽  
David S. Stevenson ◽  
Peter Wind ◽  
Massimo Vieno

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.


2019 ◽  
Vol 24 (4) ◽  
pp. 445-489
Author(s):  
Susanne Wagner

Abstract Situated at the interface of several sub-disciplines (corpus linguistics, World Englishes, variationist sociolinguistics), this study investigates patterns of adjectival amplification (very good, so glad, pretty cool) in the Corpus of Global Web-Based English (GloWbE). It highlights regional distributions/preferences of amplifier-adjective 2-grams and the idiosyncratic status of certain bigrams according to their frequency status. Globally, clear regional preferences in amplification patterns as well as possible trends concerning change are identified. Regionally, L1 varieties contrast starkly with some regions (Africa, Indian subcontinent) but – maybe unexpectedly – not with others (Southeast Asia). The results offer insights into current trajectories of change concerning the investigated amplifiers in certain regions and 2-grams: North American varieties are leading a trend away from very towards so and possibly pretty in the future.


2017 ◽  
Vol 17 (19) ◽  
pp. 11971-11989 ◽  
Author(s):  
Jun-Wei Xu ◽  
Randall V. Martin ◽  
Andrew Morrow ◽  
Sangeeta Sharma ◽  
Lin Huang ◽  
...  

Abstract. Black carbon (BC) contributes to Arctic warming, yet sources of Arctic BC and their geographic contributions remain uncertain. We interpret a series of recent airborne (NETCARE 2015; PAMARCMiP 2009 and 2011 campaigns) and ground-based measurements (at Alert, Barrow and Ny-Ålesund) from multiple methods (thermal, laser incandescence and light absorption) with the GEOS-Chem global chemical transport model and its adjoint to attribute the sources of Arctic BC. This is the first comparison with a chemical transport model of refractory BC (rBC) measurements at Alert. The springtime airborne measurements performed by the NETCARE campaign in 2015 and the PAMARCMiP campaigns in 2009 and 2011 offer BC vertical profiles extending to above 6 km across the Arctic and include profiles above Arctic ground monitoring stations. Our simulations with the addition of seasonally varying domestic heating and of gas flaring emissions are consistent with ground-based measurements of BC concentrations at Alert and Barrow in winter and spring (rRMSE  < 13 %) and with airborne measurements of the BC vertical profile across the Arctic (rRMSE  = 17 %) except for an underestimation in the middle troposphere (500–700 hPa).Sensitivity simulations suggest that anthropogenic emissions in eastern and southern Asia have the largest effect on the Arctic BC column burden both in spring (56 %) and annually (37 %), with the largest contribution in the middle troposphere (400–700 hPa). Anthropogenic emissions from northern Asia contribute considerable BC (27 % in spring and 43 % annually) to the lower troposphere (below 900 hPa). Biomass burning contributes 20 % to the Arctic BC column annually.At the Arctic surface, anthropogenic emissions from northern Asia (40–45 %) and eastern and southern Asia (20–40 %) are the largest BC contributors in winter and spring, followed by Europe (16–36 %). Biomass burning from North America is the most important contributor to all stations in summer, especially at Barrow.Our adjoint simulations indicate pronounced spatial heterogeneity in the contribution of emissions to the Arctic BC column concentrations, with noteworthy contributions from emissions in eastern China (15 %) and western Siberia (6.5 %). Although uncertain, gas flaring emissions from oilfields in western Siberia could have a striking impact (13 %) on Arctic BC loadings in January, comparable to the total influence of continental Europe and North America (6.5 % each in January). Emissions from as far as the Indo-Gangetic Plain could have a substantial influence (6.3 % annually) on Arctic BC as well.


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