Nested-grid simulation of mercury over North America

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 dom...

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Príomhchruthaitheoirí: Y. Zhang, L. Jaeglé, A. van Donkelaar, R. V. Martin, C. D. Holmes, H. M. Amos, Q. Wang, R. Talbot, R. Artz, S. Brooks, W. Luke, T. M. Holsen, D. Felton, E. K. Miller, K. D. Perry, D. Schmeltz, A. Steffen, R. Tordon, P. Weiss-Penzias, R. Zsolway
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Teanga:English
Foilsithe / Cruthaithe: Copernicus Publications 2012-07-01
Sraith:Atmospheric Chemistry and Physics
Rochtain ar líne:http://www.atmos-chem-phys.net/12/6095/2012/acp-12-6095-2012.pdf
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author Y. Zhang
L. Jaeglé
A. van Donkelaar
R. V. Martin
C. D. Holmes
H. M. Amos
Q. Wang
R. Talbot
R. Artz
S. Brooks
W. Luke
T. M. Holsen
D. Felton
E. K. Miller
K. D. Perry
D. Schmeltz
A. Steffen
R. Tordon
P. Weiss-Penzias
R. Zsolway
author_facet Y. Zhang
L. Jaeglé
A. van Donkelaar
R. V. Martin
C. D. Holmes
H. M. Amos
Q. Wang
R. Talbot
R. Artz
S. Brooks
W. Luke
T. M. Holsen
D. Felton
E. K. Miller
K. D. Perry
D. Schmeltz
A. Steffen
R. Tordon
P. Weiss-Penzias
R. Zsolway
author_sort Y. Zhang
collection DOAJ
description 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 (<i>r</i>) 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%.
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spelling doaj.art-11d09d4dfe9a4037ad1ae2ac52b51a042022-12-22T00:49:16ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242012-07-0112146095611110.5194/acp-12-6095-2012Nested-grid simulation of mercury over North AmericaY. Zhang0L. Jaeglé1A. van Donkelaar2R. V. Martin3C. D. Holmes4H. M. Amos5Q. Wang6R. Talbot7R. Artz8S. Brooks9W. Luke10T. M. Holsen11D. Felton12E. K. Miller13K. D. Perry14D. Schmeltz15A. Steffen16R. Tordon17P. Weiss-Penzias18R. Zsolway19Department of Atmospheric Sciences, University of Washington, Seattle, WA, USADepartment of Atmospheric Sciences, University of Washington, Seattle, WA, USADepartment of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, CanadaDepartment of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, CanadaDepartment of Earth System Sciences, University of California, Irvine, CA, USADepartment of Earth and Planetary Sciences, Harvard University, Cambridge MA, USASchool of Engineering and Applied Sciences, Harvard University, Cambridge MA, USADepartment of Earth and Atmospheric Sciences, University of Houston, Houston, TX, USANOAA Air Resources Laboratory, Silver Spring, MD, USANOAA Air Resources Laboratory, Silver Spring, MD, USANOAA Air Resources Laboratory, Silver Spring, MD, USADepartment of Civil and Environmental Engineering, Clarkson University, Potsdam, NY, USANew York State Department of Environmental Conservation, Division of Air Resources, Albany, NY, USAEcosystems Research Group, Norwich, VT, USADepartment of Atmospheric Sciences, University of Utah, Salt Lake City, UT, USAOffice of Atmospheric Programs, US Environmental Protection Agency, Washington DC, USAEnvironment Canada, Air Quality Research Division, Toronto, Ontario, CanadaEnvironment Canada, Air Quality Research Division, Toronto, Ontario, CanadaDepartment of Microbiology and Environmental Toxicology, University of California, Santa Cruz, CA, USADivision of Environmental Regulation, Bureau of Air Quality Monitoring, New Jersey Department of Environmental Protection, Trenton, NJ, USAWe 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 (<i>r</i>) 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%.http://www.atmos-chem-phys.net/12/6095/2012/acp-12-6095-2012.pdf
spellingShingle Y. Zhang
L. Jaeglé
A. van Donkelaar
R. V. Martin
C. D. Holmes
H. M. Amos
Q. Wang
R. Talbot
R. Artz
S. Brooks
W. Luke
T. M. Holsen
D. Felton
E. K. Miller
K. D. Perry
D. Schmeltz
A. Steffen
R. Tordon
P. Weiss-Penzias
R. Zsolway
Nested-grid simulation of mercury over North America
Atmospheric Chemistry and Physics
title Nested-grid simulation of mercury over North America
title_full Nested-grid simulation of mercury over North America
title_fullStr Nested-grid simulation of mercury over North America
title_full_unstemmed Nested-grid simulation of mercury over North America
title_short Nested-grid simulation of mercury over North America
title_sort nested grid simulation of mercury over north america
url http://www.atmos-chem-phys.net/12/6095/2012/acp-12-6095-2012.pdf
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