Updated Emission Inventories for Speciated Atmospheric Mercury from Anthropogenic Sources in China

Transcription

1 Supporting Information for: Updated Emission Inventories for Speciated Atmospheric Mercury from Anthropogenic Sources in China Lei Zhang 1,*, Shuxiao Wang 1,,*,, Long Wang 1, Ye Wu 1,, Lei Duan 1,, Qingru Wu 1, Fengyang Wang 1, Mei Yang 1, Hai Yang 1, Jiming Hao 1,, Xiang Liu 1 1 School of Environment, and State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University, Beijing 10008, China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing 10008, China Corresponding author. Tel.: ; fax: address: shxwang@tsinghua.edu.cn (S. Wang). 1 *Joint first author. These authors contributed equally to this work pages (including cover page) 7 Tables (S1, S, S, S, S, S, S7) Figures (S1, S, S, S, S, S) 17 18

2 Previous inventories for the atmospheric mercury emissions in China Table S1 shows the total Hg emissions and the uncertainty levels for anthropogenic sources in China from previous studies. Table S1 Previous researches on inventories for the atmospheric mercury emissions from anthropogenic sources in China Inventory year Source type Amount (t) Uncertainty Reference 1999 Anthropogenic sources ±% Streets et al. (00) 000 Anthropogenic sources 0 Pacyna et al. (00) 00 a) Anthropogenic sources 9 ±% Wu et al. (00) 00 Anthropogenic sources 8 ±0% Pacyna et al. (010) 007 Anthropogenic sources 09 ±0% b) Pirrone et al. (010) 199 Coal combustion 9 Feng and Hong (199) 199 Coal combustion 1 Wang et al. (1999) 000 Coal combustion 1 c) 0 c) Jiang et al. (00) 007 d) Coal combustion 0 Tian et al. (010) 010 Coal combustion ( %, +%) Zhang (01) 00 e) Non-coal sources 9 Wang et al. (00) 00 Non-ferrous metal smelting 8. Hylander and Herbert (008) 00 f) Zinc smelting 10. Li et al. (010) 00 Zinc smelting Yin et al. (01) 010 g) Non-ferrous metal smelting 010 h) municipal solid waste incineration 010 i) municipal solid waste incineration 010 municipal solid waste incineration 7. ±8% Wu et al. (01).7 Tian et al. (01).1 Hu et al. (01).7 Chen et al. (01) Notes: a) inventories for were developed, but only the 00 inventory is listed; b) the uncertainty was for the global inventory, since the uncertainty for the China inventory was not mentioned; c) using different mercury contents of coal; d) inventories for were developed, but only the 007 inventory is listed; e) inventories for were developed, but only the 00 inventory is listed; f) inventories for were developed, but only the 00 inventory is listed; g) inventories for 000, 00, 00, 007, 010 were developed, but only the 010 inventory is listed; h) inventories for were developed, but only the 010 inventory is listed; i) inventories for were developed, but only the 010 inventory is listed. S1

3 Methods for the four tiers of emission sources In the current version of the CAME model, mercury emission sources in this model were divided into categories and subcategories (Table S), and the methods for the four tiers were as follows: (1) Tier 1 uses the detailed results from existing literatures, including the data for biomass fuel combustion from Zhang et al. (01) and the data for intentional use of mercury from the Report of National Mercury Investigation of China; () Tier covers most of the emission sectors and uses the deterministic emission factor model with one single emission factor for the calculation of mercury emission from each sector; () Tier, including non-power coal combustion, non-ferrous metal smelting and cement production, adopts the technology-based probabilistic emission factor model; () Tier has only the subcategory of coal-fired power plants as far, adopting the coal-quality-regarded probabilistic emission factor model which takes into account the influence of coal quality (e.g. chlorine content) on the mercury removal efficiencies by APCDs. It should be noted that: (1) Artisanal and small-scale zinc, lead and copper smelting was included in the non-ferrous metal smelting sector; () Artisanal and small-scale gold mining (ASGM) is prohibited in China. The proportion of illegal ASGM in gold production was very low in China (e.g. 1 % in 010). The estimation was made by experts from China Gold Association; () The sector of mercury production includes primary and secondary production; () The sector of chlor-alkali production mainly includes the whole lifecycle of PVC production (including VCM production). Caustic soda production using mercury has been eliminated in China since 00. References: Zhang, W.; Wei, W.; Hu, D.; Zhu, Y.; Wang, X. J. Emission of speciated mercury from residential biomass fuel combustion in China. Energ. Fuel. 01, 7 (11), Ministry of Environmental Protection of China (MEP). Report for National Mercury Investigation of China; MEP: Beijing, China, 01. S

4 8 Table S. Categories of mercury emission sources in China and technology breakdown Unintentional use Combustion process Category Subcategory Tier Coal combustion Other combustion Coal-fired power plants Industrial coal combustion Residential coal combustion Other coal combustion Stationary oil combustion Mobile oil combustion Biomass fuel combustion 1 Municipal solid waste incineration Cremation S Type of boiler/process SF PC CFB SF PC CFB RD SF PC CFB SF PC CFB APCD combination CYC WS ESP FF ESP+WFGD FF+WFGD SCR+ESP+WFGD SCR+FF+WFGD CYC WS ESP FF ESP+WFGD FF+WFGD SCR+ESP+WFGD SCR+FF+WFGD CYC WS ESP FF ESP+WFGD FF+WFGD SCR+ESP+WFGD SCR+FF+WFGD CYC WS ESP FF ESP+WFGD FF+WFGD SCR+ESP+WFGD SCR+FF+WFGD Non-technology-based

5 Production process Non-ferrous metal smelting Precious metal production Building material production Zinc smelting Lead smelting Copper smelting Large-scale gold production Artisanal and small-scale gold mining Mercury production Cement production S EP EZF RZSP ISP AZSP RPSP SMP ISP SPP ALSP FFSP RPSP RLEP IFSP EFSP RFSP DC+FGS+ESD+DCDA DC+FGS+ESD+MRT+DCDA DC+FGS+ESD+SCSA DC+FGS DC FGS None DC+FGS+ESD+DCDA DC+FGS+ESD+MRT+DCDA DC+FGS+ESD+SCSA DC+FGS DC FGS None DC+FGS+ESD+DCDA DC+FGS+ESD+MRT+DCDA DC+FGS+ESD+SCSA DC+FGS DC FGS None Non-technology-based Shaft kiln/rotary kiln technology without dust recycling Dry-process precalciner technology with dust recycling Iron and steel production Non-technology-based Aluminum production Non-technology-based Chlor-alkali production 1 Reagent production 1 Intentional use Thermometer production 1 Non-technology-based Fluorescent lamp production 1 Battery production 1 Notes: CYC cyclone; WS wet scrubber; ESP electrostatic precipitator; FF fabric filter; WFGD wet flue gas desulfurization; CFB-FGD circulating fluidized bed flue gas desulfurization; SCR selective catalytic reduction; EP electrolytic process; RZSP retort zinc smelting process; EZF electric zinc furnace; RPSP rich-oxygen pool smelting process; ISP imperial sinter process; SMP sinter machine process; SPP sinter pan/pot process; FFSP flash furnace smelting process; IFSP imperial furnace smelting process; RLEP roasting-leaching-electrolyzing process; EFSP electric furnace smelting process; RFSP revelatory furnace smelting process; AZSP artisanal zinc smelting process; ALSP - artisanal lead smelting process; DC dust collector; FGS flue gas scrubber; ESD electrostatic demister; MRT mercury reclaiming tower; DCDA double conversion double absorption; SCSA single conversion single absorption.

6 Mercury emission factors for the mercury emission sources in Tier Emission factors for the mercury emission sources in Tier are listed in Table S. Table S. Emission factors for mercury emission sources in Tier Emission source Emission factor S Unit Reference Stationary oil combustion 1 g/t Wu et al. (00) Mobile oil combustion 8 g/t Wu et al. (00) Municipal solid waste incineration 0. g/t UNEP (00) Cremation 1.0 g/corpse UNEP (00) Large-scale gold production g/g Pacyna et al. (010) Artisanal and small-scale gold mining.0 g/g CCICED (011) Mercury production.0 g/kg UNEP (00) Iron and steel production g/t Pacyna et al. (010) Aluminum production 0. g/t TU (00) References: Wu, Y.; Wang, S. X.; Streets, D. G.; Hao, J. M.; Chan, M.; Jiang, J. K. Trends in anthropogenic mercury emissions in China from 199 to 00. Environ. Sci. Technol. 00, 0 (17), United Nations Environment Programme (UNEP). Toolkit for Identification and Quantification of Mercury Releases; UNEP Chemicals Branch: 00. Pacyna, E. G.; Pacyna, J. M.; Sundseth, K.; Munthe, J.; Kindbom, K.; Wilson, S.; Steenhuisen, F.; Maxson, P. Global emission of mercury to the atmosphere from anthropogenic sources in 00 and projections to 00. Atmos. Environ. 010, (0), China Council for International Cooperation on Environment and Development (CCICED). Special Policy Study on Mercury Management in China. CCICED, 011. Tsinghua University (TU). Improve the Estimates of Anthropogenic Mercury Emissions in China; United Nations Environment Programme (UNEP): Geneva, Switzerland, 00.

7 Mercury concentration in fuel/raw material Mercury concentration data of 8 raw coal samples, zinc concentrate samples, 190 lead concentrate samples, 17 copper concentrate samples and 17 limestone samples (for cement production) were collected from our previous studies (Zhang et al., 01; Wu et al, 01; Yang, 01). Mercury concentrations in fuel/raw material as mined by province are shown in Table S. Inter-provincial transport matrices for coal and non-ferrous metal concentrates were also derived from our previous studies (Zhang et al., 01; Wu et al, 01) to convert mercury concentrations in coal and metal concentrates as mined into mercury concentrations in coal and metal concentrates as consumed, respectively. The arithmetic mean mercury concentration in coal as consumed is 0.17 mg/kg. The arithmetic means of mercury concentrations in zinc, lead and copper concentrates as consumed are 8 mg/kg, mg/kg and. mg/kg, respectively, while the geometric means are only 0 mg/kg, 0 mg/kg and. mg/kg, respectively. The geometric mean of mercury concentration in limestone is mg/kg. With the batch fit function of the software Crystal Ball TM, the mercury concentrations in coal, metal concentrates and limestone were all found to fit the lognormal distribution References: Zhang, L.; Wang, S. X.; Meng, Y.; Hao, J. M. Influence of mercury and chlorine content of coal on mercury emissions from coal-fired power plants in China. Environ. Sci. Technol. 01, (11), 8 9. Wu, Q. R.; Wang, S. X.; Zhang, L.; Song, J. X.; Yang, H.; Meng, Y. Update of mercury emissions from China's primary zinc, lead and copper smelters, Atmos. Chem. Phys. 01, 1, Yang, H. Study on atmospheric mercury emission and control strategies from cement production in China. M.S. thesis, Tsinghua University, Beijing, 01. S

8 Table S. Mercury concentrations in fuel/raw material as mined by province (mg/kg) Coal Zn concentrate Pb concentrate Cu concentrate Limestone NS AM GM SD NS AM GM SD NS AM GM SD NS AM GM SD NS AM GM SD Anhui Beijing Chongqing Fujian Gansu Guangdong Guangxi Guizhou Hainan Hebei Heilongjiang Henan Hubei Hunan Inner Mongolia Jiangsu Jiangxi Jilin Liaoning Ningxia Qinghai Shaanxi Shandong Shanghai Shanxi Sichuan Tianjin Xinjiang Xizang Yunnan Zhejiang Imported National Note: NS number of samples; AM arithmetic mean; GM geometric mean; SD standard deviation. S7

9 . Mercury speciation in exhausted flue gas Table S shows the mercury speciation in exhausted flue gases from the dominant emission sources in China, including coal combustion, non-ferrous metal smelting, cement production and iron and steel production. Different APCD combinations will result in different speciation profiles. Mercury speciation data for other sources was inherited from previous studies (Streets et al., 00; Wu et al., 00; Zhang et al., 01), which was also shown in Table S. Table S. Mercury speciation in exhausted flue gas (%) Source type APCD combination Hg 0 Hg II Hg p No. of tests None (8-9) (-8) 10 (1-8) 1 ESP 8 (1-9) 1 (-8) 1. (0.1-10) 1 ESP+WFGD 8 (7-9) 1 (-) 0. ( ) 7 Coal combustion FF 0 (-) 9 (-7) 0. ( ) WS (9-87) (10-0).0 (0.-.) SCR+ESP+WFGD 7 (1-9) (-8) 0. (0.1-0.) FF+WFGD (CFB boiler+)esp DC+FGS+ESD+DCDA (-8) 9 (-8) DC+FGS+ESD+MRT+DCDA 90 1 Non-ferrous metal smelting DC+FGS+ESD+SCSA DC+FGS 1 1 DC (-91) (9-98) FGS (9-87) (10-0).0 (0.-.) Cement production Dry-process precalciner technology with dust recycling (9-9) 7 (1-91) 0. (0.1-1.) Shaft kiln/rotary kiln technology without dust recycling S8

10 Iron and steel production Coking+Sintering(+ESP+WFGD)+Blasting (7-1) (9-7) 0.1 Stationary oil combustion Mobile oil combustion Biomass fuel combustion 7 1 Municipal solid waste incineration 9 0 Other sources Cremation 9 0 Large-scale gold production 80 1 Artisanal and small-scale gold mining 80 1 Mercury production 80 1 Aluminum production 80 1 Intentional use References: 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 007, 8 (), Zhou, J.; Zhang, L.; Luo, Z.; Hu, C. Study on mercury emission and its control for boiler of 00 MW unit. Therm. Power Gener. 008, 7 (), 7. Wang, Y.; Duan, Y.; Yang, L.; Jiang, Y. An analysis of the factors exercising an influence on the morphological transformation of mercury in the flue gas of a 00 MW coal-fired power plant. J. Eng. Therm. Energ. Power 008, (), Yang, X.; Duan, Y.; Jiang, Y.; Yang, L. Research on mercury form distribution in flue gas and fly ash of coal-fired boiler. Coal Sci. Technol. 007, (1), 8. Duan, Y.; Cao, Y.; Kellie, S.; Liu, K.; Riley, J. T.; Pan, W. In-situ measurement and distribution of flue gas mercury for a utility PC boiler system. J. Southeast Univ. 00, 1 (1), 7. S9

11 Kellie, S.; Duan, Y.; Cao, Y.; Chu, P.; Mehta, A.; Carty, R.; Liu, K.; Pan, W.; Riley, J. T. Mercury emissions from a 100-MW wall-fired boiler as measured by semicontinuous mercury monitor and Ontario Hydro Method. Fuel Process. Technol. 00, 8 ( 7), Shah, P.; Strezov, V.; Nelson, P. Speciation of mercury in coal-fired power station flue gas. Energ. Fuel. 010,, 0 1. Guo, X.; Zheng, C.; Jia, X.; Lin, Z.; Liu, Y. Study on mercury speciation in pulverized coal-fired flue gas. P. CSEE 00, (), Tang, S. The mercury species and emissions from coal combustion flue gas and landfill gas in Guiyang. Ph.D. thesis, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, 00. Goodarzi, F. Speciation and mass-balance of mercury from pulverized coal fired power plants burning western Canadian subbituminous coals. J. Environ. Monit. 00, (10), Lee, S. J.; Seo, Y. C.; Jang, H. N.; Park, K. S.; Baek, J. I.; An, H. S.; Song, K. C. Speciation and mass distribution of mercury in a bituminous coal-fired power plant. Atmos. Environ. 00, 0 (1), 1. Kim, J. H.; Pudasainee, D.; Yoon, Y. S.; Son, S. U.; Seo, Y. C. Studies on speciation changes and mass distribution of mercury in a bituminous coal-fired power plant by combining field data and chemical equilibrium calculation. Ind. Eng. Chem. Res. 010, 9, Zhang, L.; Wang, S. X.; Meng, Y.; Hao, J. M. Influence of mercury and chlorine content of coal on mercury emissions from coal-fired power plants in China. Environ. Sci. Technol. 01, (11), 8 9. Wang, S. X.; Zhang, L.; Li, G. H.; Wu, Y.; Hao, J. M.; Pirrone, N.; Sprovieri, F.; Ancora, M. P. Mercury emission and speciation of coal-fired power plants in China. Atmos. Chem. Phys. 010, 10 (), Zhang, L. Emission characteristics and synergistic control strategies of atmospheric mercury from coal combustion in China. Ph.D. thesis, Tsinghua University, Beijing, 01. Zhang, L.; Wang, S. X.; Wu, Q. R.; Meng, Y.; Yang, H.; Wang, F. Y.; Hao, J. M. Were mercury emission factors for Chinese non-ferrous metal smelters overestimated? Evidence from onsite measurements in six smelters. Environ. Pollut. 01, 171, S10

12 Wu, Q. R.; Wang, S. X.; Zhang, L.; Song, J. X.; Yang, H.; Meng, Y. Update of mercury emissions from China's primary zinc, lead and copper smelters, Atmos. Chem. Phys. 01, 1, Wang, S. X.; Song, J. X.; Li, G. H.; Wu, Y.; Zhang, L.; Wan, Q.; Streets, D. G.; Chin, C. K. Estimating mercury emissions from a zinc smelter in relation to China's mercury control policies. Environ. Pollut. 010, 18 (10), 7. Li, G. H.; Feng, X. B.; Li, Z. G.; Qiu, G. L.; Shang, L. H.; Liang, P.; Wang, D. Y.; Yang, Y. K. Mercury emission to atmosphere from primary Zn production in China. Sci. Total Environ. 010, 08 (0), Wang, F. Y.; Wang, S. X.; Zhang, L.; Yang, H.; Wu, Q. R.; Hao, J. M. Mercury enrichment and its effects on atmospheric emissions in cement plants of China. Atmos. Environ. 01, 9, 1 8. Li, W. J. Characterization of atmospheric mercury emissions from coal-fired power plant and cement plant. M.S. thesis, Southwest University, Chongqing, 011. Streets, D. G.; Hao, J. M.; Wu, Y.; Jiang, J. K.; Chan, M.; Tian, H. Z.; Feng, X. B. Anthropogenic mercury emissions in China. Atmos. Environ. 00, 9 (0), Wu, Y.; Wang, S. X.; Streets, D. G.; Hao, J. M.; Chan, M.; Jiang, J. K. Trends in anthropogenic mercury emissions in China from 199 to 00. Environ. Sci. Technol. 00, 0 (17), Zhang, W.; Wei, W.; Hu, D.; Zhu, Y.; Wang, X. J. Emission of speciated mercury from residential biomass fuel combustion in China. Energ. Fuel. 01, 7 (11), S11

13 7 8. Activity levels and APCD application rates of mercury emission sources in China Table S shows the activity levels of different mercury emission sources in China. It should be noted that the activity level of non-ferrous metal smelting was converted from the amount of metal product to the amount of metal concentrate consumed based on the grade of the concentrate (0%, % and % for Zn, Pb and Cu respectively) and the metal recovery rate (9%, 9% and 97% for Zn, Pb and Cu respectively). The activity level of cement production was converted from the amount of clinker to that of limestone used based on the limestone/clinker ratio (1.). Table S7 shows the application rates of APCD combinations in major Hg emission sources in China in 000, 00 and 010. Table S. Activity levels of mercury emission sources in China, Emission source Fuel/product Unit AAGR a Coal-fired power plants Coal Mt % Industrial coal combustion Coal Mt % Residential coal combustion Coal Mt % Other coal combustion Coal Mt % Stationary oil combustion Oil Mt % Mobile oil combustion Oil Mt % Waste incineration Waste Mt % Cremation Corpse million % Zinc smelting Zinc kt % Lead smelting Lead kt % Copper smelting Copper kt % Gold production Gold t % Mercury production Mercury t % Cement production Cement Mt % Iron and steel production Pig steel Mt % Aluminum production Aluminum Mt % Notes: a Annual average growth rate. S1

14 Table S7. Application rates of APCD combinations in major Hg emission sources in China in 010 (%) Emission source APCD combination Emission source APCD combination Coal-fired power plants CYC WS ESP FF ESP+WFGD FF+WFGD SCR+ESP+WFGD SCR+FF+WFGD Zinc smelting DC+FGS+ESD+DCDA DC+FGS+ESD+MRT+DCDA DC+FGS+ESD+SCSA DC+FGS DC FGS None None 1.0 CYC.0 DC+FGS+ESD+DCDA WS DC+FGS+ESD+MRT+DCDA Industrial coal combustion ESP FF ESP+WFGD Lead smelting DC+FGS+ESD+SCSA DC+FGS DC FF+WFGD.0 FGS SCR+ESP+WFGD None SCR+FF+WFGD DC+FGS+ESD+DCDA Cement production Shaft kiln/rotary kiln technology without dust recycling Dry-process precalciner technology with dust recycling Copper smelting DC+FGS+ESD+MRT+DCDA DC+FGS+ESD+SCSA DC+FGS DC FGS None S1

15 7. Methodology for uncertainty analysis Figure S1 shows a general skewed distribution. The P10 P90 range only reflects the span of the skewed distribution, and fails to embody the kurtosis of the distribution which largely affects the uncertainty range. f(mo) f(mo)/ σ s σ k σ k + σ s u P0 Mo σ k Mo P0 u + Mo+σ k + P80 Figure S1. Characteristic parameters of a general skewed distribution The uncertainty range of general statistical data can be described by relative standard deviation (RSD): u σ =± (S1) µ where u is the uncertainty, σ is the standard deviation; and µ is the mean value. For normal distribution, Equation (S1) is also applicable, and the mean value (µ) is meanwhile P0 value and mode (Mo) as well. The probability at the position of µ is: 1 f ( µ ) = (S) πσ The probability f(µ) or f(mo) is the maximum value in the probabilistic distribution. Given that σ s is the distance from µ or Mo to the value where the probability equals to f(µ)/ or f(mo)/, there is: 1 f ( µ ± σ s ) = (S) πσ Based on Equation (S), we can get that σ s equals to 1.18σ. Given σ k is the distance from µ or Mo to P0 or P80, we can get that σ k equals to 0.8σ. It can be seen that σ s S1

16 and σ k reflect the span and the kurtosis of the distribution, respectively, and there is: s k = (S) σ σ σ Therefore, the uncertainty of a normal distribution can also be expressed as: u σ σ s k =± (S) µ Expanding the application of Equation (S) to the general skewed distribution (see Figure S1), the distances from Mo to the values where the probability equal to f(mo)/ (σ s and σ + s ), the distances from Mo to P0 and P80 (σ k and σ + k ) reflect the span of the distribution, and the best estimate for the distribution is the P0 value. Eventually we get the positive and negative uncertainty as follows: u Mo σ sσ k = 1 (S) P0 Mo σ + sσ k u = 1 (S7) P0 This approach for uncertainty analysis fits the normal distribution case and is better to compare with previous studies, e.g. Streets et al. (00). P10/P90 ranges from the study of Wu et al. (010) can be better referred as the confidence interval with a confidence degree of 80% References: Streets, D. G.; Hao, J. M.; Wu, Y.; Jiang, J. K.; Chan, M.; Tian, H. Z.; Feng, X. B. Anthropogenic mercury emissions in China. Atmos. Environ. 00, 9 (0), Wu, Y.; Streets, D. G.; Wang, S. X.; Hao, J. M. Uncertainties in estimating mercury emissions from coal-fired power plants in China. Atmos. Chem. Phys. 010, 10, S1

17 8. Anthropogenic mercury emissions in China from 000 to 010 Figure S summarizes the trend of total atmospheric mercury emissions in China. Figure S shows the sectoral distribution of mercury emissions in China in 010. Total atmospheric mercury emission (t) 00 Intentional use Aluminum production Iron and steel production 00 Cement production Mercury production Artisanal and small-scale gold mining 00 Large-scale gold production Copper smelting Lead smelting 00 Zinc smelting Cremation Municipal solid waste incineration 00 Biomass fuel combustion Mobile oil combustion Stationary oil combustion 100 Other coal combustion Residential coal combustion Industrial coal combustion 0 Coal-fired power plants Figure S. Trend of total atmospheric mercury emission in China, Mercury production 1% Iron and steel production % Aluminum production 1% Intentional use 1% Artisanal and small-scale gold mining 1% Cement production 18% Coal-fired power plants 19% 7 Large-scale gold production % Copper smelting 1% Lead smelting % Municipal solid waste incineration % Cremation 1% Zinc smelting 1% Biomass fuel combustion 1% Mobile oil combustion % Industrial coal combustion % Stationary oil combustion 0% Residential coal combustion % Other coal combustion % Figure S. Sectoral distribution of mercury emissions in China in 010 S1

18 Figure S shows the trends of thermal electric power generation and Hg emissions from coal-fired power plants Thermal electric power generation (billion kwh) Electricity generation Hg emissions Hg emission from coal-fired power plants (t) Year Figure S. Trends of thermal electric power generation and Hg emissions from coal-fired power plants in China Figure S shows the trends of mercury emissions from dominant sources Sectoral atmospheric mercury emission (t) Coal-fired power plants Industrial coal combustion Non-ferrous metal smelting Cement production Figure S. Trends of mercury emissions from dominant sources in China S17

19 9. Gridded mercury emissions from different sources in China in 010 Figure S shows the gridded mercury emissions from four dominant anthropogenic sources in China in 010. S18

20 (a) (b) Power Plants Unit: kg Non-ferrous Unit: kg (c) (d) 1 Cement Unit: kg Figure S. Gridded mercury emissions from different sources in China in 010: (a) coal-fired power plants; (b) non-ferrous metal Iron Unit: kg smelting; (c) cement production; (d) iron and steel production S19