ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-2937-2010 Uncertainties in estimating mercury emissions from coal-fired power plants in China Wu Y. 1 Streets D. G. 2 Wang S. X. 1 Hao J. M. 1 Department of Environmental Science and Engineering, and State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University, Beijing 100084, China Decision and Information Sciences Division, Argonne National Laboratory, Argonne, Illinois 60439, USA 29 03 2010 10 6 2937 2946 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/10/2937/2010/acp-10-2937-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/2937/2010/acp-10-2937-2010.pdf

A detailed multiple-year inventory of mercury emissions from anthropogenic activities in China has been developed. Coal combustion and nonferrous metals production continue to be the two leading mercury sources in China, together contributing ~80% of total mercury emissions. However, many uncertainties still remain in our knowledge of primary anthropogenic releases of mercury to the atmosphere in China. In situations involving large uncertainties, our previous mercury emission inventory that used a deterministic approach could produce results that might not be a true reflection of reality; and in such cases stochastic simulations incorporating uncertainties need to be performed. Within our inventory, a new comprehensive sub-module for estimation of mercury emissions from coal-fired power plants in China is constructed as an uncertainty case study. The new sub-module integrates up-to-date information regarding mercury content in coal by province, coal washing and cleaning, coal consumption by province, mercury removal efficiencies by control technology or technology combinations, etc. Based on these detailed data, probability-based distribution functions are built into the sub-module to address the uncertainties of these key parameters. The sub-module incorporates Monte Carlo simulations to take into account the probability distributions of key input parameters and produce the mercury emission results in the form of a statistical distribution. For example, the best estimate for total mercury emissions from coal-fired power plants in China in 2003 is 90.5 Mg, with the uncertainty range from 57.1 Mg (P10) to 154.6 Mg (P90); and the best estimate for elemental mercury emissions is 43.0 Mg, with the uncertainty range from 25.6 Mg (P10) to 75.7 Mg (P90). The results further indicate that the majority of the uncertainty in mercury emission estimation comes from two factors: mercury content of coal and mercury removal efficiency.

 References China Power Industry: 2004 China Power Yearbook. China Power Press, Beijing, China, 2004. Banic, C. M., Beauchamp, S. T., Tordon, R. J., Schroeder, W. H., Steffen, A., Anlauf, K. A., and Wong, H. K. T.: Vertical distribution of gaseous elemental mercury in Canada. J. Geophys. Res., 108(D9), 4264, doi:10.1029/2002JD002116, 2003. Brinkman, N., Wang, M., Weber, T., and Darlington, T.: Well-to-wheels analysis of advanced fuel/vehicle systems-a North American study of energy use, greenhouse gas emissions, and criteria pollutant emissions. Online available at: http://www.transportation.anl.gov/software/GREET/publications.html, 2005. Chen, L.; Duan, Y.; Zhuo, Y.; Yang, L.; Zhang, L.; Yang, X.; Yao, Q.; Jiang, Y.; Xu, X.: Mercury transformation across particulate control devices in six power plants of China: The co-effect of chlorine and ash composition. Fuel, 86(4), 603–610, 2007. Dastoor, A. P. and Larocque, Y.: Global circulation of atmospheric mercury: a modeling study. Atmos. Environ., 38, 147–161, 2004. 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, 2005. Fang, F., Wang, Q., Liu, R., Ma, Z., and Hao, Q.: Atmospheric particulate mercury in Changchun City, China, Atmos. Environ. 35, 4265–4272, 2001. Fu, X., Feng, X., Wang, S., Rothenberg, S., Shang, L., Li, Z., and Qiu, G.: Temporal and spatial distributions of total gaseous mercury concentrations in ambient air in a mountainous area in southwestern China: Implications for industial and domestic mercury emissions in remote areas in China, Sci. Total Environ., 407, 2306–2314, 2009. Fu, X. W., Feng, X., Dong, Z. Q., Yin, R. S., Wang, J. X., Yang, Z. R., and Zhang, H.: Atmospheric gaseous elemental mercury (GEM) concentrations and mercury depositions at a high-altitude mountain peak in south China, Atmos. Chem. Phys., 10, 2425–2437, 2010. Feng, X., Sommer, J., Lindqvist, O., and Hong, Y.: Occurrence, emissions and deposition of mercury during coal combustion in the province Guizhou, China, Water Air Soil Pollut., 139, 311–324, 2002. Feng, X., Tang, S., Shang, L., Yan, H., Sommar, J., and Lindqvist, O.: Total gaseous mercury in the atmosphere of Guiyang, PR China, Sci. Total Environ., 304, 61–72, 2003. Feng, X., Shang, L., Wang, S., Tang, S., and Zheng, W.: Temporal variation of total gaseous mercury in the air of Guiyang, China, J. Geophys. Res., 109, D03303, doi:10.1029/2003JD004159, 2004a. Feng, X., Yan, H., Wang, S., Qiu, G., Tang, S., Shang, L., Dai, Q., and Hou, Y.: 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.: Mercury pollution in China – an overview. In: Dynamics of Mercury Pollution on Regional and Global Scales: Atmospheric Processes, Human Exposure Around the World, edited by: Pirrone, N. and Mahaffey, K. Springer Publishers, Norwell, MA, USA, 657–678, 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., 109, D19S25, doi:10.1029/2003JD004244, 2004. Huang, W. and Yang, Y.: Mercury in coal in China. Coal Geology of China, 14(S), 37–40, 2002. Lindberg, S., Bullock, R., Ebinghaus, R., Engstrom, D., Feng, X., 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(1), 19–32, 2007. Liu, S., Nadim, F., Perkins, C., Carley, R. J., Hoag, G. E., Lin, Y., and Chen, L.: Atmospheric mercury monitoring survey in Beijing, China, Chemosphere, 48, 97–107, 2002. National Bureau of Statistics of China, P.R. China: China Energy Statistical Yearbook (2003). China Statistics Press, Beijing, China, 2005. Pacyna, J. M. and Pacyna, E. G.: Global emissions of mercury to the atmosphere. Emissions from anthropogenic sources; Arctic Monitoring and Assessment Programme (AMAP), Oslo, Norway, 1996. Pacyna, E. G. and Pacyna, J. M.: Global emission of mercury from anthropogenic sources in 1995. Water Air Soil Pollut., 137, 149–165, 2002. 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., 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., 111, D07109, doi:10.1029/2005JD006381, 2006. Seigneur, C., Karamchandani, P., Lohman, K., Vijayaraghavan, K., and Shia, R.-L.: Multiscale modeling of the atmospheric fate and transport of mercury, J. Geophys. Res., 106(D21), 27795–27809, 2001. 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(2), 555–569, 2004. Steding, D. J. and Flegal, A. R.: Mercury concentrations in coastal California precipitation: evidence of local and trans-Pacific fluxes of mercury to North America. J. Geophys. Res., 107(D24), 4764, doi:10.1029/2002JD002081, 2002. 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., 112, D02308, doi:10.1029/2006JD007450, 2007. Srivastava, R. K., Hutson, N., Martin, B., and Princiotta, F.: Control of mercury emissions from coal-fired electric utility boilers. Environ. Sci. Technol., 40(5), 1385–1393, 2006. Streets, D. G., Bond, T. C., Carmichael, G. R., Fernandes, S. D., Fu, Q., He, D., Klimont, Z., Nelson, S. M., Tsai, N. Y., Wang, M. Q., Woo, J.-H., and Yarber, K. F.: An inventory of gaseous and primary aerosol emissions in Asia in the year 2000. J. Geophys. Res., 108(D21), 8809, doi:10.1029/2002JD003093, 2003a. Streets, D. G., Yarber, K. F., Woo, J.-H., and Carmichael, G. R.: Biomass burning in Asia: Annual and seasonal estimates and atmospheric emissions, Global Biogeochem. Cy., 17(4), 1099, doi:10.1029/2003GB002040, 2003b. 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. Streets, D. G., Hao, J., Wang, S., and Wu, Y.: Mercury emissions from coal combustion in China, in Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications, edited by: Pirrone, N. and Mason, R., United Nations Environment Programme, 2008. Subramanyan, K., Wu, Y., Diwekar, U. M., and Wang, M. Q.: New stochastic simulation capability applied to the GREET model. Int. J. LCA., 13(3), 278–285, 2008. Travnikov, O. and Ryaboshapko, A.: Modelling of Mercury Hemispheric Transport and Depositions. MSC-E Technical Report 6/2002. Meteorological Synthesizing Centre-East, Moscow, Russia, 67 pp., 2002. US Geological Survey (USGS): Mercury content in coal mines in China (unpublished data), 2004. US Environmental Protection Agency (US EPA): Mercury Study Report to Congress, Volume II: An Inventory of Anthropogenic Mercury Emissions in the United States, EPA-452/R-97-004, 1997. US Environmental Protection Agency (US EPA): Research and Development: Characterization and Management of Residues from Coal-fired Power Plants, EPA-600/R-02-083, 2002. 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, 2007. Wan, Q., Feng, X., Lu, J., Zheng, W., Song, X., Han, S., 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, 2009. Wang, Q., Shen, W., and Ma, Z.: Estimation of mercury emission from coal combustion in China, Environ. Sci. Technol., 34, 2711–2713, 2000. Wang, S. X., Zhang, L., Li, G. H., Wu, Y., Hao, J. M., Pirrone, N., Sprovieri, F., and Ancora, M. P.: Mercury emission and speciation of coal-fired power plants in China, Atmos. Chem. Phys., 10, 1183–1192, 2010a. Wang, S. X., Zhang, L., Wu, Y., Ancora, M. P., Zhao, Y., and Hao, J. M.: Synergistic mercury removal by conventional pollutant control strategies for coal-fired power plants in China, J. Air Waste Manage. Assoc., 60, doi:10.3155/1047-3289.60.5.1, 2010b. 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, 2006. Zhang, J., Ren, D., Xu, D., and Zhao, F.: Mercury in coal and its effect on environment, Adv. Environ. Sci., 7(3), 100–104, 1999. Zhang, L., Zhuo, Y., Chen, L., Xu, X., and Chen, C.: Mercury emissions from six coal-fired power plants in China, Fuel Process. Technol., 89(11), 1033–1040, 2008. Zhou, J., Zhang, L., Luo, Z., and Hu, C.: Study on mercury emission and its control for boiler of 300 MW unit. Thermal Power Generation, 37(4), 22–27, 2008. Zhu, Z., Xu, L., and Tan, Y.: Research on characteristics of mercury distribution in combustion products for a 300MW pulverized coal fired boiler, Power Eng., 22, 1594–1597, 2002.