Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 10 1 2010 10.5194/acpd-10-1383-2010 http://www.atmos-chem-phys-discuss.net/10/1383/2010/ http://www.atmos-chem-phys-discuss.net/10/1383/2010/acpd-10-1383-2010.html http://www.atmos-chem-phys-discuss.net/10/1383/2010/acpd-10-1383-2010.pdf 1383 1416 2010-01-20 Mercury air-borne emissions from 5 municipal solid waste landfills in Guiyang and Wuhan, China Z. G. Li X. Feng fengxinbin@vip.skleg.cn P. Li L. Liang S. L. Tang S. F. Wang X. W. Fu G. L. Qiu L. H. Shang State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China Cebam Analytical, Inc., 3927 Aurora Avenue N, Seattle, WA 98103, USA A detailed study on atmospheric mercury emissions from municipal solid waste (MSW) landfills in China is necessary to understand mercury behavior in this source category, simply because China disposes of bulk MSW by landfilling and a large quantity of mercury enters into landfills. Between 2003 and 2006, mercury airborne emissions through different pathways, as well as mercury speciation in landfill gas (LFG) were measured at 5 MSW landfills in Guiyang and Wuhan, China. The results showed that mercury content in the substrate fundamentally affected the magnitude of mercury emissions, resulting in the highest emission rate (as high as 57 651 ng Hg m^−2 h^−1) at the working face and in un-covered waste areas, and the lowest measured at soil covers and vegetation areas (less than 20 ng Hg m^−2 h^−1). Meteorological parameters, especially solar radiation, influenced the diurnal pattern of mercury surface-air emissions. Total gaseous mercury (TGM) in LFG varied from 2.0 to 1406.0 ng m^−3, monomethyl mercury (MMHg) and dimethyl mercury (DMHg) in LFG averaged at 1.93 and 9.21 ng m^−3, and accounted for 0.51% and 1.79% of the TGM in the LFG, respectively. Total mercury emitted from the five landfills ranged from 17 to 3285 g yr^−1, with the highest from the working face, then soil covering, and finally the vent pipes. Bloom,~N S., Grout,~A K., and Prestbo,~E M.: Development and complete validation of a~method for the determination of dimethyl mercury in air and other media, Anal. Chim. Acta, 546(1), 92–101, 2005. de la Rosa,~D A., Velasco,~A., Rosas,~A., and Volke-Sep\'ulveda,~T.: Total gaseous mercury and volatile organic compounds measurements at five municipal solid waste disposal sites surrounding the Mexico city metropolitan area, Atmos. Environ., 40(12), 2079–2088, 2006. Fang,~M. and Liu,~H.: Investigation and experiments on the control of heavy metal pollutants in dumping grounds in Wuhan, China Environ. Sci., 8(4), 55–59, 1988 (in Chinese with abstract in English). Feldmann,~J., Grümping,~R., and Hirner,~A V.: Determination of volatile metal and metalloid compounds in gases from domestic waste deposits with GC-ICP-MS, Fresenius J. Anal. Chem., 350(4–5), 228–235, 1994. Feng,~X., Li,~G., and Qiu,~G.: A~preliminary study on mercury contamination to the environment from artisanal zinc smelting using indigenous methods in Hezhang county, Guizhou, China – Part~1: mercury emission from zinc smelting and its influences on the surface waters, Atmos. Environ., 38(36), 6223–6230, 2004a. 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, \doi10.1029/2003JD004159, 2004b. Feng,~X., Wang,~S., Qiu,~G., Hou,~Y., and Tang,~S.: Total gaseous mercury emissions from soil in Guiyang, Guizhou, China, J Geophys. Res., 110, D14306, \doi10.1029/2004JD005643, 2005. Gebert,~J. and Groengroeft,~A.: Passive landfill gas emission-Influence of atmospheric pressure and implications for the operation of methane-oxidising biofilters, Waste Manage., 26(3), 245–251, 2006. Gustin,~M S., Lindberg,~S E., Austin,~K., Coolbaugh,~M., Vette,~A., and Zhang,~H.: Assessing the contribution of natural sources to regional atmospheric mercury budgets, Sci. Total Environ., 259(1–3), 61–71, 2000. Hao,~C. and Shen,~Y.: Study on production and mercury consumption of clinical mercury-thermometers in China, Res. Environ. Sci., 19(1), 18–21, 2006 (in Chinese with abstract in English). Hawkins,~L. and Prestbo,~E.: Dimethyl mercury in municipal waste landfill gas: measurements and analytical method development, in: Proceedings of the 7th International Conference on Mercury as Global Pollutant, Ljubljana, 28~June–2~July 2004. Huang,~Q., Wang,~Q., Dong,~L., Xi,~B., and Zhou,~B.: The current situation of solid waste management in China, J Mater. Cycles Waste, 8(1), 63–69, 2006. Huang,~Y. and He,~Q.: Study on the status of output and utilization of landfill gas in China, J Sichuan Univ. Sci. & Eng. (Nat. Sci. Ed.), 21(1), 117–120, 2008 (in Chinese with abstract in English). Jian,~X., Shen,~Y., and Cao,~G.: Investigation of mercury usage in the battery production and recommended reduced countermeasures, Environ. Sci. Manage., 33(10), 10–13, 2008 (in Chinese with abstract in English). Kim,~K H., Kim,~M Y., and Lee,~G.: The soil-air exchange characteristics of total gaseous mercury from a~large scale municipal landfill area, Atmos. Environ., 35(20), 3475–3493, 2001. Kim,~K H. and Kim,~M Y.: Mercury emissions as landfill gas from a~large-scale abandoned landfill site in Seoul, Atmos. Environ., 36(31), 4919–4928, 2002. Kim,~K H., Choi,~Y J., Jeon,~E C., and Sunwoo,~Y.: Characterization of malodorous sulfur compounds in landfill gas, Atmos. Environ., 39(6), 1103–1112, 2005. Li,~G., Feng,~X., Li,~Z.: Atmospheric mercury emissions from retort Zn productions, J Tsinghua Univ. (Sci. & Tech.), 49(12), 2001–2004, 2009 (in Chinese with abstract in English). Lindberg,~S E. and Price,~J.: Airborne emissions of mercury from municipal landfill operations: a~short-term measurement study in Florida, J Air Waste Manage., 49(5), 520–532, 1999. Lindberg,~S E., Wallschlager,~D., Prestbo,~E M., Bloom,~N S., Price,~J L., and Reinhart,~D.: Methylated mercury species in municipal waste landfill gas sampled in Florida, USA, Atmos. Environ., 35(23), 4011–4015, 2001. Lindberg,~S E., Southworth,~G., Prestbo,~E M., Wallschläger,~D., Bogle,~M A., and Price,~J.: Gaseous methyl- and inorganic mercury in landfill gas from landfills in Florida, Minnesota, Delaware, and California, Atmos. Environ., 39(2), 249–258, 2005a. Lindberg,~S E., Southworh,~G R., Bogle,~M A., Blasing,~T J., Owens,~J., Roy,~K., Zhang,~H., Kuiken,~T., Price,~J., Reinhart,~D., and Sfeir,~H.: Airborne emissions of mercury from municipal solid waste, 1: new measurements from six operating landfills in Florida, J Air Waste Manage., 55(7), 859–869, 2005b. Liu,~J., Liu,~J., and Xu,~W. : Review and outlook on MSW sanitary landfill technology in China, Environ. Sanit. Eng., 15(4), 58–61, 2007 (in Chinese with abstract in English). Maurice,~C. and Lagerkvist,~A.: LFG emission measurements in cold climatic conditions: seasonal variations and methane emissions mitigation, Cold Reg. Sci. Technol., 36(1–3), 37–46, 2003. Munthe,~J., Wangberg,~I., Iverfeldt,~A., Lindqvist,~O., Stromberg,~D., Sommar,~J., Gardfeldt,~K., Petersen,~G., Ebinghaus,~R., Prestbo,~E., Larjava,~K., and Siemens,~V.: Distribution of atmospheric mercury species in Northern Europe: final results from the MOE project, Atmos. Environ., 37(Sup 1), S9–S20, 2003. Nierenberg,~D W., Nordgren,~R E., Chang,~M B., Siegler,~R W., Blayney,~M B., Hochberg,~F., Toribara,~T Y., Cernichiari,~E., and Clarkson,~T.: Delayed cerebellar disease and death after accidental exposure to dimethylmercury, New Engl J. Med., 338(23), 1672–1676, 1998. OECD: Sector case studies: household energy and water consumption and waste generation: trends, environmental impacts and policy responses. (ENV/EPOC/WPNEP(2001)15/FINAL) Organization for Economic Cooperation and Development Environment Directorate 1999–2001 Programme on Sustainable Development, Paris, France, 56–83, 2001. Poissant,~L. and Casimir,~A.: Water-air and soil-air exchange rate of total gaseous mercury measured at background sites, Atmos. Environ., 32(5), 883–893, 1998. Prestbo,~E M., Hawkins,~L., Cussen,~D., and Fowler,~C.: Determination of total and dimethyl mercury in raw landfill gas with site screening for elemental mercury at eight Washington state landfills for the Washington State Department of Ecology, Frontier Geosciences Inc, online available at http://www.ecy.wa.gov/mercury/documents/Mercury_landfill_gas.pdf, 2003. Shen,~Y. and Jian,~X.: Mercury consumption abatement in China, Res. Environ. Sci., 17(3), 13–15, 2004 (in Chinese with abstract in English). Tang,~S., Feng,~X., Qiu,~J., Yin,~G., and Yang,~Z.: Mercury speciation and emissions from coal combustion in Guiyang, southwest China, Environ. Res., 105, 175–182, 2007. Tekran: Model 2357A – Principles of operation, Tekran Inc. Toronto, Canada, 1998. Sommar,~J., Feng,~X., and Lindqvist,~O.: Speciation of volatile mercury species present in digester and deposit gases, Appl. Organomet. Chem., 13(6), 441–445, 1999. US EPA: Characterization of products containing mercury in municipal solid waste in the US, 1970–2000, EPA530-S-92–013, US Government Printing Office, Washington, DC, 1992. US EPA: User's guide for the industrial source complex (ISC3) dispersion models, Volume I-user instructions, Washington, DC, 1995. US EPA: Mercury study report to congress, Volume~2: An inventory of anthropogenic mercury emissions in the United States, United States Environmental Protection Agency EPA-452/R-97-004, Office of Air Quality Planning and Standards & Office of Research and Development, NC, Dec 1997. van Velzen,~D., Langenkamp,~H., and Herb,~G.: Review: mercury in waste incineration, Waste Manage. Res., 20(6), 556–568, 2002. Wang,~Q., Shen,~W., and Ma,~Z.: Estimation of mercury emission from coal combustion in China, Environ. Sci. Technol., 34(13), 2711–2713, 2000. Wang,~J.: Study of environmental geochemical baseline of pollutional heavy metals in surficial soil of Guiyang, Guizhou, Doctor dissertation of Institute of Geochemistry, Chinese Academy of Sciences, 2004 (in Chinese with abstract in English). Wang,~S., Feng,~X., Qiu,~G., and Fu,~X.: Comparison of air/soil mercury exchange between warm and cold season in Hongfeng reservoir region, Environ. Sci., 25(1), 123–127, 2004 (in Chinese with abstract in English). Wang,~S., Feng,~X., Qiu,~G., Wei,~Z., and Xiao,~T.: Mercury emission to atmosphere from Lanmuchang Hg-Tl mining area, Southwestern Guizhou, China, Atmos. Environ., 39(39), 7459–7473, 2005. Wang,~S., Zhang,~L., Li,~G., Wu,~Y., Hao,~J., Pirrone,~N., Sprovieri,~F., and Ancora,~M P.: Mercury emission and speciation of coal-fired power plants in China, Atmos. Chem. Phys. Discuss., 9, 24051–24083, 2009. Wu,~Y., Wang,~S., Streets,~D G., Hao,~J., Chan,~M., and Jiang,~J.: Trends in anthropogenic mercury emissions in China from 1995 to 2003, Environ. Sci. Technol., 40(17), 5312–5318, 2006. Yang,~F., Liu,~J., and Wang,~R.: Estimation on the amount of mercury used in domestic batteries and potential amount of mercury emissions in China, Shanghai Environ. Sci., 22(5), 322–328, 2003 (in Chinese with abstract in English). Yu,~Y. and Li,~J.: Recovery and disposal of waste battery in China, Sichuan Environ., 23(1), 94–96, 2004 (in Chinese with abstract in English).