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1 Supporting Information for Anthropogenic Emissions of Hydrogen Chloride and Fine Particulate Chloride in China Xiao Fu a, *, Tao Wang a, *, Shuxiao Wang b, c, Lei Zhang d, Siyi Cai b, Jia Xing b, Jiming Hao b, e a Department of Civil and Environmental Engineering, Hong Kong Polytechnic University, Hong Kong 99907, China b State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing , China c State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing , China d School of the Environment, Nanjing University, 163 Xianlin Ave., Nanjing, Jiangsu , China e Collaborative Innovation Center for Regional Environmental Quality, Tsinghua University, Beijing , China * Correspondence to: Tao Wang (tao.wang@polyu.edu.hk) and Xiao Fu (x.fu@polyu.edu.hk ) Number of pages: 11 Number of Tables: 4 Number of Figures: 2 S1

2 Table S1. Emission source categorization. Sector Subsector Technology/Process Power plants Stoker furnace/pulverized coal boiler/circulating fluidized bed boiler Coal combustion Domestic combustion Stoker furnace/stove Industrial boilers Stoker furnace/pulverized coal boiler/circulating fluidized bed boiler Cement clinker production Precalciner kilns/shaft kilns/other rotary kilns Iron-steel production Sinter/puddling Industrial processes Lime production Brick production HCl production Biomass burning Open burning Different crop straw Household burning Different crop straw, firewood Forest/grass wild fires Different vegetation types MSW incineration Open burning Incineration plants Grated firing incinerator/fluidized bed incinerator S2

3 Table S2. Key characteristics of distribution functions for Cl content in raw coal produced in major provinces in China (ppm) Provinces Number of samples Distribution P5 * P50 * P95 * Mean Anhui 27 Lognormal Guizhou 49 Lognormal Hebei 24 Beta Heilongjiang 20 Lognormal Henan 45 Lognormal Inner Mongolia 55 Lognormal Liaoning 22 Lognormal Shaanxi 29 Lognormal Shandong 35 Lognormal Shanxi 93 Beta Sichuan 19 Lognormal Xinjiang 20 Lognormal Yunnan 17 Lognormal China 537 Lognormal * P5 values mean that there is a probability of 5% that the actual values would be equal to or below the P5 values; P50 mean that there is a probability of 50% that the actual values would be equal to or below the P50 values; and P95 mean that there is a probability of 95% that the actual values would be equal to or below the P95 values S3

4 Table S3. Cl percentages in PM 2.5 emissions from different sources. Source category Control Devices Cl percentage in PM 2.5 emission (%) Reference pulverized coal boiler SCR+ESP+FF+WFGD 1.75 Ref. 1 pulverized coal boiler SCR+FF+WFGD 1.85 Ref. 2 pulverized coal boiler SCR+ESP+WFGD 0.2 Ref. 3 pulverized coal boiler SCR+ESP+WFGD 0.69 Ref. 4 pulverized coal boiler SCR+ESP+WFGD 3 Ref. 5 pulverized coal boiler ESP+WFGD 0.6 Ref. 5 pulverized coal boiler ESP+WFGD 0.68 Ref. 4 pulverized coal boiler FF 1.12 Ref. 6 pulverized coal boiler FF 0.72 Ref. 6 pulverized coal boiler ESP+FF 0.72 Ref. 6 pulverized coal boiler FF 1.22 Ref. 6 pulverized coal boiler CYC+ESP 1.32 Ref. 6 pulverized coal boiler ESP 0.4 Ref. 7 circulating fluidized bed boiler HED+CFB-FGD 1 Ref. 3 circulating fluidized bed boiler FF+CFB-FGD 0.61 Ref. 8 circulating fluidized bed boiler FF+CFB-FGD 0.33 Ref. 5 circulating fluidized bed boiler ESP+CFB-FGD 1.15 Ref. 8 circulating fluidized bed boiler ESP+WFGD 0.62 Ref. 9 circulating fluidized bed boiler WET 0.19 Ref. 10 circulating fluidized bed boiler NOC 0.81 Ref. 8 circulating fluidized bed boiler NOC 0.9 Ref. 8 stoker furnace FF+WFGD 4.97 Ref. 8 stoker furnace FF+WFGD 8.23 Ref. 11 stoker furnace FF+WFGD 0.18 Ref. 11 stoker furnace FF+WFGD 7.13 Ref. 11 stoker furnace FF+WFGD 0.45 Ref. 1 stoker furnace HED+WFGD 0.55 Ref. 2 stoker furnace WET+WFGD 4.75 Ref. 8 stoker furnace WET+WFGD 0.81 Ref. 12 stoker furnace WET+WFGD 1.09 Ref. 12 stoker furnace WET+WFGD 5.85 Ref. 11 stoker furnace FF 7.5 Ref. 8 stoker furnace FF 1.35 Ref. 11 stoker furnace FF 5.61 Ref. 11 stoker furnace ESP 2.03 Ref. 10 stoker furnace WET 0.73 Ref. 10 stoker furnace WET 1.17 Ref. 10 stoker furnace WET 7.63 Ref. 8 stoker furnace WET 7.94 Ref. 11 stoker furnace WET Ref. 11 S4

5 stoker furnace WET 12.7 Ref. 11 stoker furnace WET 1.72 Ref. 10 stoker furnace CYC 2.53 Ref. 12 stoker furnace CYC 1.44 Ref. 10 stoker furnace CYC 3.97 Ref. 10 stoker furnace NOC 2.73 Ref. 8 stoker furnace NOC 0.44 Ref. 11 stoker furnace NOC 2.83 Ref. 8 stoker furnace NOC 2.48 Ref. 11 stoker furnace NOC 8.5 Ref. 11 stoker furnace NOC 1.22 Ref. 11 stoker furnace NOC 0.38 Ref. 11 stoker furnace NOC 2.64 Ref. 11 stove NOC 0.64 Ref. 13 stove NOC 1 Ref. 7 Sinter production ESP+Dry-FGD 20 Ref. 4 Sinter production ESP+WFGD 3.11 Ref. 14 Sinter production ESP+WFGD 3.22 Ref. 15 Sinter production ESP+WFGD 0.74 Ref. 15 Sinter production ESP+WFGD 5.85 Ref. 15 Sinter production ESP 1.39 Ref. 15 Sinter production ESP 3.87 Ref. 15 Sinter production ESP 7.94 Ref. 15 Sinter production ESP 8.37 Ref. 16 Sinter production ESP 1.5 Ref. 7 Puddling FF 2.49 Ref. 4 Puddling FF 1.53 Ref. 14 Puddling FF 6.59 Ref. 16 Precalciner clinker kilns FF 0.3 Ref. 7 Precalciner clinker kilns FF 1.72 Ref. 17 Shaft clinker kilns SNCR+FF 0.16 Ref. 2 Wheat-household burning Ref. 18 Wheat-household burning 8.11 Ref. 18 Wheat-household burning 15 Ref. 19 Wheat-open burning Ref. 20 Wheat-open burning 1.91 Ref. 21 Wheat-open burning 10 Ref. 19 Wheat-open burning 6.08 Ref. 22 Wheat-open burning 7.21 Ref. 22 Wheat-open burning 8.82 Ref. 23 Corn-household burning Ref. 18 Corn-household burning Ref. 18 Corn-open burning Ref. 20 Corn-open burning 5.98 Ref. 22 S5

6 Corn-open burning Ref. 23 Rice-household burning 5.58 Ref. 18 Rice-household burning Ref. 19 Rice-open burning Ref. 19 Rice-open burning 3.23 Ref. 23 Rape-household burning 14 Ref. 19 Rape-open burning 7.53 Ref. 21 Rape-open burning 19 Ref. 19 Cotton-household burning 0.84 Ref. 18 Soybean-household burning 4.39 Ref. 18 Soybean-household burning Ref. 19 Soybean-open burning 6.64 Ref. 19 sorghum-household burning 1.63 Ref. 18 Firewood-household burning 1.46 Ref. 18 Firewood-household burning 3.14 Ref. 18 Firewood-household burning 1.65 Ref. 18 Firewood-household burning 4.74 Ref. 18 S6

7 Table S4. Assumptions for uncertainty analysis. Parameters Distribution Activity Data Power plants Normal (CV: 5%) Domestic combustion Normal (CV: 20%) Industrial boilers Normal (CV: 10%) Iron & steel production Normal (CV: 5%) Cement production Normal (CV: 10%) Brick production Normal (CV: 10%) Lime production Normal (CV: 10%) Biomass burning Normal (CV: 30%) MSW incineration Normal (CV: 10%) MSW open burning Normal (CV: 30%) Release rate Pulverized coal boiler Uniform (78%, 93%) Stoker furnace Uniform (75%, 85%) Circulating fluidized bed boiler Uniform (86%, 93%) Stove Weibull (Data fitting) HCl Removal efficiency Wet scrubber Uniform (40%, 60%) ESP Uniform (0.9%, 12%) FF Uniform (9.5%, 11.3%) WFGD Uniform (93%, 99.4%) Other-FGD Uniform (85%, 94%) HCl emission factor Cement kiln (g/t) Uniform (5.37, 37.15) Sinter production (g/t) Lognormal (CV: 50%) Lime kiln (g/t) Lognormal (CV: 50%) Brick kiln (g/t) Lognormal (CV: 50%) Biomass burning - rice straw (g/kg) Uniform (0.0393,0.8065) Biomass burning - wheat straw (g/kg) Uniform (0.0201,1.0034) Biomass burning - sugar cane straw (g/kg) Uniform (0.0446,0.1321) Biomass burning - other crop straw (g/kg) Lognormal (CV: 50%) Biomass burning wild fires (g/kg) Lognormal (CV: 50%) Biomass burning firewood (g/kg) Uniform (0.0376,0.087) MSW incineration - grated firing incinerator (g/kg) Uniform (0.0761, ) MSW incineration - fluidized bed incinerator (g/kg) Uniform (0.089,0.0891) MSW open burning (g/kg) Lognormal (CV: 50%) HCl production (g/kg) Lognormal (CV: 50%) Fine particle Cl- percentage Pulverized coal boiler Uniform (0.2%, 3%) Stoker furnace Exponential (Data fitting) Circulating fluidized bed boiler Uniform (0.19%, 1.15%) S7

8 Stove Uniform (0.64%, 1%) Sinter production Uniform (0.74%, 20%) Puddling Uniform (1.53%, 6.59%) Cement kiln Uniform (0.16%, 1.72%) Lime kiln Lognormal (CV: 50%) Brick kiln Lognormal (CV: 50%) Biomass burning-wheat straw Uniform (1.91%, 16.86%) Biomass burning-corn straw Uniform (5.98%, 23.01%) Biomass burning-rice straw Uniform (3.23%, 29.37%) Biomass burning-rape straw Uniform (7.53%, 19%) Biomass burning-soybean straw Uniform (4.39%, 14.01%) Biomass burning-other crop straw Lognormal (CV: 50%) Biomass burning-wild fires Lognormal (CV: 50%) Biomass burning-firewood Uniform (1.46%, 4.74%) MSW burning Lognormal (CV: 50%) S8

9 Figure S1 Spatial distribution of chlorine emission intensity (HCl + Cl -, kg Cl/km 2 ) in RCEI data and this study. S9

10 PM 2.5 _Cl - concentration (µg/m 3 ) obs sim_this study sim_rcei_1990 3/5 3/6 3/7 3/8 3/9 3/10 3/11 3/12 3/13 3/14 3/15 3/16 3/17 3/18 3/19 3/20 3/21 3/22 3/23 3/24 3/25 3/26 3/27 3/28 3/29 3/30 3/31 4/1 4/2 4/3 4/4 4/5 Figure S2. Comparison of observed and simulated PM 2.5 _Cl - concentrations at Changchun site based on the chlorine emissions from RCEI_1990 and this study. Reference: 1. Liang, Y.; Wang, Z.; Ma, Z.; Shi, A.; Hu, Y.; Wang, C.; Yang, D., Study on the particle matter emission characteristics of flue gas from coal-fired boilers equipped with wet desulphurization. Environmental Monitoring in China 2016, 5, Ma, Z.; Liang, Y.; Zhang, J.; Zhang, D.; Shi, A.; Hu, J.; Lin, A.; Feng, Y.; Hu, Y.; Liu, B., PM2.5 profiles of typical sources in Beijing. Acta Chim. Sinica. 2015, 35, Ma, Z.; Li, Z.; Jiang, J.; Ye, Z.; Deng, J.; Duan, L., Characteristics of Water-Soluble Inorganic Ions in PM2. 5 Emitted from Coal Fired Power Plants. Environm. Sci. 2015, 36, Zheng, M.; Zheng, Y.; Yan, C.; Fu, H.; Niu, H.; Huang, K.; Hu, M.; Zeng, L.; Liu, Q.; Pei, B.; Fu, Q., Establishing PM2.5 industrial source profiles in Shanghai. China Environm. Sci. 2013, 33, Pei, B.; Wang, X. L.; Zhang, Y. H.; Hu, M.; Sun, Y. J.; Deng, J.; Dong, L.; Fu, Q. Y.; Yan, N. Q., Emissions and source profiles of PM2.5 for coal-fired boilers in the Shanghai megacity, China. Atmospheric Pollution Research 2016, 7, Wang, Y.; Peng, L.; Wang, Y.; Zhang, T.; Liu, H.; Mu, L., Characteristics of Chemical Components in PM2. 5 from the Coal Dust of Power Plants. Environm. Sci. 2016, 37, Kong, S. PM source profile, and risk assessment and emissions of hazardous pollutants. Doctorial Thesis, Nankai University, Tianjin, Liu, X. RESEARCH ON FINE PARTICULATE MATTER GENERATION AND EMISSION CHARACTERISTICS OF LAYER BURNING BOILERS AND FLUIDIZED BED BOILER FOR HEATING-SUPPLY. Master Thesis, Harbin Institute of Technology, Harbin, S10

11 9. Zhao, L.; Zhang, D.; Zhou, Z.; Ren, L.; Yin, B.; Yuan, R., A study on emission characteristics of particulate matters from typical industrial combustion sources in Chongqing city. Journal of Environmental Engineering Technology 2015, 5, Li, C.; Li, X.; Duan, L.; Zhao, M.; Duan, J.; Hao, J., Emission Characteristics of PM10 from Coal-Fired Industrial Boiler. Environm. Sci. 2009, 3, Cao, Y. RESEARCH ON PM2.5 PRODUCTION AND EMISSION CHARACTERISTICS OF LAYER BURNING BOILERS FROM HEATING-SUPPLY INDUSTRY. Master Thesis, Harbin Institute of Technology, Harbin, Shang, Y. RESEARCH ON LAYER BURNING INDUSTRIAL BOILER PM2.5 EMISSIONS CHARACTERISTICS. Master Thesis, Harbin Institute of Technology, Harbin, Zhang, H. F.; Wang, S. X.; Hao, J. M.; Wan, L.; Jiang, J. K.; Zhang, M.; Mestl, H. E. S.; Alnes, L. W. H.; Aunan, K.; Mellouki, A. W., Chemical and size characterization of particles emitted from the burning of coal and wood in rural households in Guizhou, China. Atmos. Environ. 2012, 51, Zhao, H. The emissions characteristic and reduction strategies study on PM2.5 of ferrous metal smelting(steel) industry. Master Thesis, North China Electric Power University, Beijing, Wang, Y. RESEARCH ON PM2.5 PRODUCTION AND EMISSION CHARACTERISTICS OF IRON AND STEEL SINTERING MACHINE. Master Thesis, Hebei University of Technology, Tianjin, Ma, J. Emission characteristics of particulates from typical production process of iron and steel enterprises. Master Thesis, Southwest University, Chongqing, Ma, J. Research on Emission Characteristics of Air Pollutants from Cement Industry. Master Thesis, Hebei University of engineering, Handan, Li, X. H.; Duan, L.; Wang, S. X.; Duan, J. C.; Guo, X. M.; Yi, H. H.; Hu, J. N.; Li, C.; Hao, J. M., Emission characteristics of particulate matter from rural household biofuel combustion in China. Energ. Fuel. 2007, 21, Tang, X.; Huang, C.; Lou, S.; Qiao, L.; Wang, H.; Zhou, M.; Chen, M.; Chen, C.; Wang, Q.; Li, G.; Li, L.; Huang, H.; Zhang, G., Emission factors and PM chemical composition study of biomass burning in the Yangtze River Delta Region. Environm.Sci 2014, 35, Li, X. G.; Wang, S. X.; Duan, L.; Hao, J.; Li, C.; Chen, Y. S.; Yang, L., Particulate and trace gas emissions from open burning of wheat straw and corn stover in China. Environ. Sci. Technol. 2007, 41, Du, H. Tracer components in the PM emissions from wheat and rape straw combustion. Master Thesis, Nankai University, Tianjin, Wang, Y.; Hu, M.; Wang, Y.; Qin, Y.; Chen, H.; Zeng, L.; Lei, J.; Huang, X.; He, L.; Zhang, R.; Wu, Z., Characterization and Influence Factors of PM2.5 Emitted from Crop Straw Burning. Acta Chim. Sinica. 2016, 74, Deng, C. Identification of biomass burning source in aerosols and the formation mechanism of haze. Doctorial Thesis, Fudan University, Shanghai, S11

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

Supporting Information for: Updated Emission Inventories for Speciated Atmospheric Mercury from Anthropogenic Sources in China 7 8 9 10 11 Lei Zhang 1,*, Shuxiao Wang 1,,*,, Long Wang 1, Ye Wu 1,, Lei