Atmospheric Chemistry and Physics Discussions
www.atmos-chem-phys-discuss.net
1680-7367
1680-7375
9
5
2009
10.5194/acpd-9-21285-2009
http://www.atmos-chem-phys-discuss.net/9/21285/2009/
http://www.atmos-chem-phys-discuss.net/9/21285/2009/acpd-9-21285-2009.html
http://www.atmos-chem-phys-discuss.net/9/21285/2009/acpd-9-21285-2009.pdf
21285
21315
2009-10-09
Estimating mercury emission outflow from East Asia using CMAQ-Hg
C.-J. Lin
jerry.lin@lamar.edu
L. Pan
D. G. Streets
S. K. Shetty
C. Jang
X. Feng
H.-W. Chu
T. C. Ho
Department of Civil Engineering, Lamar University, Beaumont, TX 77710, USA
School of Environmental Science & Engineering, South China University of Technology, Guangzhou, 510006, Guangdong, China
Department of Mechanical Engineering, Lamar University, Beaumont, TX 77710, USA
Decision and Information Sciences Division, Argonne National Laboratory, Argonne, IL 60439, USA
Department of Chemical Engineering, Lamar University, Beaumont, TX 77710, USA
Office of Air Quality Planning and Standards, USEPA, Research Triangle Park, NC 27711, USA
State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China
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<sup>−1</sup>) and PHg (13~21 Mg mo<sup>−1</sup>), and
a net export of GEM (60~130 Mg mo<sup>−1</sup>) 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<sup>−1</sup>, 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.
Bullock, O. R. and Brehme, K. A.: Atmospheric mercury simulation using the cmaq model: Formulation description and analysis of wet deposition results, Atmos. Environ., 36, 2135–2146, 2002.
Byun, D. W. and Ching, J. K. S.: Science algorithms of the EPA Models-3 Community Multiscale Air Quality (CMAQ) modeling system. Rep EPA-600/R-99/030. Office of Research and Development, US Environmental Protection Agency, Washington, DC, 1999.
Byun, D. and Schere, K. L.: Review of the governing equations, computational algorithms, and other components of the models-3 community multiscale air quality (cmaq) modeling system, Appl. Mech. Rev., 59, 51–77, doi:10.1115/1.2128636, 2006.
Carmichael, G. R., Tang, Y., Kurata, G., Uno, I., Streets, D. G., Thongboonchoo, N., Woo, J. H., Guttikunda, S., White, A., Wang, T., Blake, D. R., Atlas, E., Fried, A., Potter, B., Avery, M. A., Sachse, G. W., Sandholm, S. T., Kondo, Y., Talbot, R. W., Bandy, A., Thorton, D., and Clarke, A. D.: Evaluating regional emission estimates using the trace-p observations, J. Geophys. Res. Atmos., 108, 8810, doi:10.1029/2002jd003116, 2003.
Chand, D., Jaffe, D., Prestbo, E., Swartzendruber, P. C., Hafner, W., Weiss-Penzias, P., Kato, S., Takami, A., Hatakeyama, S., and Kajii, Y.: Reactive and particulate mercury in the asian marine boundary layer, Atmos. Environ., 42, 7988–7996, 2008.
Choi, E. M., Kim, S. H., Holsen, T. M., and Yi, S. M.: Total gaseous concentrations in mercury in seoul, korea: Local sources compared to long-range transport from china and japan, Environ. Pollut., 157, 816–822, doi:10.1016/j.envpol.2008.11.023, 2009.
Fang, F., Wang, Q., Liu, R., Ma, Z., and Hao, Q.: Atmospheric particulate mercury in Changchun City, China, Atmos. Environ., 35, 4265–4272, 2001.
Fang, F. M., Wang, Q. C., and Li, J. F.: Urban environmental mercury in Changchun, a~metropolitan city in northeastern China: Source, cycle, and fate, Sci. Total Environ., 330, 159–170, doi:10.1016/j.scitotenv.2004.04.006, 2004.
Feng, X. B., Shang, L. H., Wang, S. F., Tang, S. L., and Zheng, W.: Temporal variation of total gaseous mercury in the air of Guiyang, China, J. Geophys. Res. Atmos., 109, D03303, doi:10.1029/2003JD004159, 2004a.
Feng, X. B., Yan, H. Y., Wang, S. F., Qiu, G. L., Tang, S. L., Shang, L. H., Dai, Q. J., and Hou, Y. M.: Seasonal variation of gaseous mercury exchange rate between air and water surface over Baihua reservoir, Guizhou, China, Atmos. Environ., 38, 4721–4732, 2004b.
Feng, X. B., Wang, S. F., Qiu, G. A., Hou, Y. M., and Tang, S. L.: Total gaseous mercury emissions from soil in Guiyang, Guizhou, China, J. Geophys. Res. Atmos., 110, D14306, doi:10.1029/2004JD005643, 2005.
Friedli, H. R., Radke, L. F., Prescott, R., Li, P., Woo, J. H., and Carmichael, G. R.: Mercury in the atmosphere around japan, korea, and china as observed during the 2001 ace-asia field campaign: Measurements, distributions, sources, and implications, J. Geophys. Res. Atmos., 109, D19S25, doi:10.1029/2003jd004244, 2004.
Fu, X. W., Feng, X. B., Zhu, W. Z., Wang, S. F., and Lu, J. L.: Total gaseous mercury concentrations in ambient air in the eastern slope of mt. Gongga, south-eastern fringe of the Tibetan plateau, China, Atmos. Environ., 42, 970–979, 2008a.
Fu, X. W., Feng, X. B., Zhu, W. Z., Zheng, W., Wang, S. F., and Lu, J. Y.: Total particulate and reactive gaseous mercury in ambient air on the eastern slope of the mt. Gongga area, China, Appl. Geochem., 23, 408–418, 2008b.
Grell, G. A., Dudhia, J., and Stauffer, D. R.: A~description of the fifth-generation Penn State/NCAR Mesoscale Model (MM5), NCAR Tech Note TN-398$+$STR, 122~pp., 1994.
Guo, Y., Feng, X., Li, Z., He, T., Yan, H., Meng, B., Zhang, J., and Qiu, G.: Distribution and wet deposition fluxes of total and methyl mercury in Wujiang river basin, Guizhou, China, Atmos. Environ., 42, 7096–7103, 2008.
Jaffe, D., Prestbo, E., Swartzendruber, P., Weiss-Penzias, P., Kato, S., Takami, A., Hatakeyama, S., and Kajii, Y.: Export of atmospheric mercury from asia, Atmos. Environ., 39, 3029–3038, doi:10.1016/j.atmosenv.2005.01.030, 2005.
Jaffe, D. and Strode, S.: Sources, fate and transport of atmospheric mercury from asia, Environ. Chem., 5, 121–126, doi:10.1071/en08010, 2008.
Kim, K. H., Ebinghaus, R., Schroeder, W. H., Blanchard, P., Kock, H. H., Steffen, A., Froude, F. A., Kim, M. Y., Hong, S. M., and Kim, J. H.: Atmospheric mercury concentrations from several observatory sites in the northern hemisphere, J. Atmos. Chem., 50, 1–24, doi:10.1007/s10874-005-9222-0, 2005.
Kim, S. H., Han, Y. J., Holsen, T. M., and Yi, S. M.: Characteristics of atmospheric speciated mercury concentrations (tgm, hg(ii) and hg(p)) in Seoul, Korea, Atmos. Environ., 43, 3267–3274, doi:10.1016/j.atmosenv.2009.02.038, 2009.
Lamborg, C. H., Fitzgerald, W. F., Vandal, G. M., and Rolfhus, K. R.: Atmospheric mercury in northern wisconsin – sources and species, Water Air Soil Pollut., 80, 189–198, 1995.
Lin, C.-J., Pongprueksa, P., Lindberg, S. E., Pehkonen, S. O., Byun, D., and Jang, C.: Scientific uncertainties in atmospheric mercury models i: Model science evaluation, Atmos. Environ., 40, 2911–2928, 2006a.
Lin, C. J. and Pehkonen, S. O.: The chemistry of atmospheric mercury: A~review, Atmos. Environ., 33, 2067–2079, 1999.
Lin, C.-J., Pongprueksa, P., Streets, D. G., Jang, C., Ho, T., and Chu, H.: Trans-Pacific Chemical Transport of Mercury: Sensitivity Analysis on Potential Asian Emission Contribution to Mercury Deposition in North America Using CMAQ-Hg. in: The 5th CMAS Conference, Research Triangle Park, NC, 16–18 October, 2006a.
Lin, C. J., Pongprueksa, P., Lindberg, S. E., Pehkonen, S. O., Byun, D., and Jang, C.: Scientific uncertainties in atmospheric mercury models 1: Model science evaluation, Atmos. Environ., 40, 2911–2928, doi:10.1016/j.atmosenv.2006.01.009, 2006b.
Lin, C. J., Pongprueks, P., Rusell Bulock, O., Lindberg, S. E., Pehkonen, S. O., Jang, C., Braverman, T., and Ho, T. C.: Scientific uncertainties in atmospheric mercury models 2: Sensitivity analysis in the conus domain, Atmos. Environ., 41, 6544–6560, doi:10.1016/j.atmosenv.2007.04.030, 2007.
Lindberg, S., Bullock, R., Ebinghaus, R., Engstrom, D., Feng, X. B., Fitzgerald, W., Pirrone, N., Prestbo, E., and Seigneur, C.: A~synthesis of progress and uncertainties in attributing the sources of mercury in deposition, Ambio, 36, 19–32, 2007.
Lindberg, S. E., Brooks, S., Lin, C. J., Scott, K. J., Landis, M. S., Stevens, R. K., Goodsite, M., and Richter, A.: Dynamic oxidation of gaseous mercury in the arctic troposphere at polar sunrise, Environ. Sci. Technol., 36, 1245–1256, doi:10.1021/es0111941, 2002.
Liu, S. L., Nadim, F., Perkins, C., Carley, R. J., Hoag, G. E., Lin, Y. H., and Chen, L. T.: Atmospheric mercury monitoring survey in Beijing, China, Chemosphere, 48, 97–107, 2002.
Mason, R. P., Morel, F. M. M., and Hemond, H. F.: The role of microorganisms in elemental mercury formation in natural-waters, Water Air Soil Pollut., 80, 775–787, 1995.
Mason, R. P. and Sheu, G. R.: Role of the ocean in the global mercury cycle, Global Biogeochem. Cy., 16, 1093, doi:10.1029/2001gb001440, 2002.
Mason, R. P., Kim, E. H., Cornwell, J., and Heyes, D.: An examination of the factors influencing the flux of mercury, methylmercury and other constituents from estuarine sediment, Mar. Chem., 102, 96–110, doi:10.1016/j.marchem.2005.09.021, 2006.
Miller, C. L., Mason, R. P., Gilmour, C. C., and Heyes, A.: Influence of dissolved organic matter on the complexation of mercury under sulfidic conditions, Environ. Toxicol. Chem., 26, 624–633, 2007.
Moussiopoulos, N., Helmis, C. G., Flocas, H. A., Louka, P., Assimakopoulos, V. D., Naneris, C., and Sahm, P.: A~modelling method for estimating transboundary air pollution in southeastern europe, Environ. Model. Softw., 19, 549–558, doi:10.1016/j.envsoft.2003.07.003, 2004.
Nguyen, H. T., Kim, K. H., Kim, M. Y., Hong, S. M., Youn, Y. H., Shon, Z. H., and Lee, J. S.: Monitoring of atmospheric mercury at a~global atmospheric watch (gaw) site on an-myun island, korea, Water Air Soil Pollut., 185, 149–164, doi:10.1007/s11270-007-9438-5, 2007.
Pacyna, E. G., Pacyna, J. M., Steenhuisen, F., and Wilson, S.: Global anthropogenic mercury emission inventory for 2000, Atmos. Environ., 40, 4048–4063, 2006.
Pan, L., Woo, J. H., Carmichael, G. R., Tang, Y. H., Friedli, H. R., and Radke, L. F.: Regional distribution and emissions of mercury in east asia: A~modeling analysis of asian pacific regional aerosol characterization experiment (ace-asia) observations, J. Geophys. Res. Atmos., 111, D07109, doi:10.1029/2005jd006381, 2006.
Pan, L., Chai, T. F., Carmichael, G. R., Tang, Y. H., Streets, D., Woo, J. H., Friedli, H. R., and Radke, L. F.: Top-down estimate of mercury emissions in china using four-dimensional variational data assimilation, Atmos. Environ., 41, 2804–2819, doi:10.1016/j.atmosenv.2006.11.048, 2007.
Pan, L., Carmichael, G. R., Adhikary, B., Tang, Y. H., Streets, D., Woo, J. H., Friedli, H. R., and Radke, L. F.: A~regional analysis of the fate and transport of mercury in east asia and an assessment of major uncertainties, Atmos. Environ., 42, 1144–1159, doi:10.1016/j.atmosenv.2007.10.045, 2008.
Pleim, J. E. and Byun, D. W.: Application of a~new land-surface, dry deposition, and PBL model in the models-3 Community Multi-Scale Air Quality (CMAQ) model system, in: Air Pollution Modeling and Its Application XIV, edited by: Gryning, S., Schiermeier, F. A., Kluwer Academic Publishers, New York, 297–305, 2004.
Pongprueksa, P., Lin, C. J., Lindberg, S. E., Jang, C., Braverman, T., Bullock, O. R., Ho, T. C., and Chu, H. W.: Scientific uncertainties in atmospheric mercury models iii: Boundary and initial conditions, model grid resolution, and hg(ii) reduction mechanism, Atmos. Environ., 42, 1828–1845, doi:10.1016/j.atmosenv.2007.11.020, 2008.
Rolfhus, K. R., Sakamoto, H. E., Cleckner, L. B., Stoor, R. W., Babiarz, C. L., Back, R. C., Manolopoulos, H., and Hurley, J. P.: Distribution and fluxes of total and methylmercury in lake superior, Environ. Sci. Technol., 37, 865–872, 2003.
Schroeder, W. H., Anlauf, K. G., Barrie, L. A., Lu, J. Y., Steffen, A., Schneeberger, D. R., and Berg, T.: Arctic springtime depletion of mercury, Nature, 394, 331–332, 1998.
Schroeder, W. H., and Munthe, J.: Atmospheric mercury – an overview, Atmos. Environ., 32, 809–822, 1998.
Seigneur, C., Vijayaraghavan, K., Lohman, K., Karamchandani, P., and Scott, C.: Global source attribution for mercury deposition in the united states, Environ. Sci. Technol., 38, 555–569, doi:10.1021/es034109t, 2004.
Selin, N. E., Jacob, D. J., Park, R. J., Yantosca, R. M., Strode, S., Jaegle, L., and Jaffe, D.: Chemical cycling and deposition of atmospheric mercury: Global constraints from observations, J. Geophys. Res. Atmos., 112, D02308, doi:10.1029/2006jd007450, 2007.
Shetty, S. K., Lin, C. J., Streets, D. G., and Jang, C.: Model estimate of mercury emission from natural sources in east asia, Atmos. Environ., 42, 8674–8685, doi:10.1016/j.atmosenv.2008.08.026, 2008.
Shia, R. L., Seigneur, C., Pai, P., Ko, M., and Sze, N. D.: Global simulation of atmospheric mercury concentrations and deposition fluxes, J. Geophys. Res. Atmos., 104, 23747–23760, 1999.
Stratton, W. J., Lindberg, S. E., and Perry, C. J.: Atmospheric mercury speciation: Laboratory and field evaluation of a~mist chamber method for measuring reactive gaseous mercury, Environ. Sci. Technol., 35, 170–177, 2001.
Streets, D. G., Hao, J. M., Wu, Y., Jiang, J. K., Chan, M., Tian, H. Z., and Feng, X. B.: Anthropogenic mercury emissions in china, Atmos. Environ., 39, 7789–7806, 2005.
Strode, S. A., Jaegle, L., Jaffe, D. A., Swartzendruber, P. C., Selin, N. E., Holmes, C., and Yantosca, R. M.: Trans-pacific transport of mercury, J. Geophys. Res. Atmos., 113, D15305, doi:10.1029/2007jd009428, 2008.
Wan, Q., Feng, X. B., Lu, J., Zheng, W., Song, X. J., Li, P., Han, S. J., and Xu, H.: Atmospheric mercury in changbai mountain area, northeastern china ii. The distribution of reactive gaseous mercury and particulate mercury and mercury deposition fluxes, Environ. Res., 109, 721–727, 2009a.
Wan, Q., Feng, X. B., Lu, J. L., Zheng, W., Song, X. J., Han, S. J., and Xu, H.: Atmospheric mercury in changbai mountain area, northeastern china i. The seasonal distribution pattern of total gaseous mercury and its potential sources, Environ. Res., 109, 201–206, 2009b.
Wang, Z. W., Zhang, X. S., Chen, Z. S., and Zhang, Y.: Mercury concentrations in size-fractionated airborne particles at urban and suburban sites in Beijing, China, Atmos. Environ., 40, 2194–2201, 2006.
Wang, Z. W., Chen, Z. S., Duan, N., and Zhang, X. S.: Gaseous elemental mercury concentration in atmosphere at urban and remote sites in China, J. Environ. Sci. China, 19, 176–180, 2007.
Weiss-Penzias, P., Jaffe, D. A., Swartzendruber, P., Dennison, J. B., Chand, D., Hafner, W., and Prestbo, E.: Observations of asian air pollution in the free troposphere at mount bachelor observatory during the spring of 2004, J. Geophys. Res. Atmos., 111, D10304, doi:10.1029/2005jd006522, 2006.
Weiss-Penzias, P., Jaffe, D., Swartzendruber, P., Hafner, W., Chand, D., and Prestbo, E.: Quantifying asian and biomass burning sources of mercury using the hg/co ratio in pollution plumes observed at the mount bachelor observatory, Atmos. Environ., 41, 4366–4379, doi:10.1016/j.atmosenv.2007.01.058, 2007.
Wu, Y., Wang, S. X., Streets, D. G., Hao, J. M., Chan, M., and Jiang, J. K.: Trends in anthropogenic mercury emissions in china from 1995 to 2003, Environ. Sci. Technol., 40, 5312–5318, doi:10.1021/es060406x, 2006.
Xiu, G. L., Cai, J., Zhang, W. Y., Zhang, D. N., Bueler, A., Lee, S. C., Shen, Y., Xu, L. H., Huang, X. J., and Zhang, P.: Speciated mercury in size-fractionated particles in shanghai ambient air, Atmos. Environ., 43, 3145–3154, 2009.
Yang, Y. K., Chen, H., and Wang, D. Y.: Spatial and temporal distribution of gaseous elemental mercury in chongqing, china, Environ. Monit. Assess., 156, 479–489, 2009.
Zender, C. S. and Mangalarn, H.: Scaling properties of common statistical operators for gridded datasets, Int. J. High Perform. C., 21, 485–498, doi:10.1177/1094342007083802, 2007.