Supporting Information. Residential Coal Combustion as a Source of Levoglucosan in China

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1 1 Supporting Information Residential Coal Combustion as a Source of Levoglucosan in China Caiqing Yan, Mei Zheng *,, Amy P. Sullivan, Guofeng Shen,a, Yingjun Chen, Shuxiao Wang, Bin Zhao, Siyi Cai, Yury Desyaterik, Xiaoying Li, Tian Zhou, Örjan Gustafsson #, Jeffrey L. Collett Jr. SKL-ESPC and BIC-ESAT, College of Environmental Sciences and Engineering and College of Urban and Environmental Sciences, Peking University, Beijing , China Department of Atmospheric Science, Colorado State University, Fort Collins, Colorado 80523, USA United States Key Laboratory of Cities Mitigation and Ada6ption to Climate Change in Shanghai (China Meteorological Administration), College of Environmental Science and Engineering, Tongji University, Shanghai , China. 15 State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing , China # Department of Environmental Science and Analytical Chemistry (ACES) and the Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden a Present Address: National Risk Management Research Laboratory (NRMRL), U.S. EPA, Research Triangle Park, North Carolina 27709, United States * Corresponding author: mzheng@pku.edu.cn 23 Pages 11 Text 1 Tables 4 Figures 3 S1

2 Table of Contents Text S1 Method for estimating levoglucosan (LG) emissions from residential solid fuels in mainland China Table S1. Summary information of solid fuels used in this study Table S2. Characteristics of the coals tested in this study Table S3. EF LG used for estimating LG emission and the fraction of LG from coal combustion (LG_Coal) to total LG from the residential solid fuel sector (LG_Total) Table S4. Ratios with the +/- standard deviation of LG to other water-soluble saccharides measured in solid fuel combustion samples and ambient samples in this study. Figure S1. Source testing system with combustion equipment and sampling system. (Note: MFC denotes mass flow controller) Figure S2. Profiles of saccharides for each type of solid fuel combustion source sample shown as box and whisker plots. Panel A. Crop straw burning samples; Panel B: Wood burning samples; Panel C: Coal combustion samples (Note: Percentage of LG here is shown as one tenth of the real value) Figure S3. LG/MN and LG/GA ratios in biomass burning and coal combustion emissions. (Note: Error bars represent one standard deviation) S2

3 Text S1 Method for estimating levoglucosan (LG) emissions from residential solid fuels in northern China To estimate the LG emissions from residential solid fuels in northern China, including provinces such as Heilongjiang, Jilin, Liaoning, Hebei, Beijing, Tianjin, Shandong, Henan, Shanxi, Shaanxi, Gansu and Qinghai, and autonomous regions such as Ningxia, Xinjiang and Inner Mongolia, the total fuel consumption of coal (e.g., coal and briquette coal) and biomass (e.g., crop straw and wood) for household heating and cooking in different provinces of northern China were considered. The data for 2013 were from previous references. 1 Based on the EF LG_coal, EF LG_crop and EF LG_wood measured in this study, the emissions of LG from residential coal and biomass burning activities in different provinces in 2013 were then roughly estimated using the following equation: E Res,p = s EF p,s,f A p,s,f (S1) Where E represents emissions (unit: t); Res is short for residential sector; p is the province in northern China; E Res, p represents emissions from residential sectors in a certain province; s is a specific sector (e.g., heating, cooking); f is the specific type of fuel; EF denotes the emission factor (unit: mg kg -1 fuel) measured in this study, and EF p,s,f is the province-specific emission factor, with consideration of fuel used in each province and associated maturity distribution of coals. A is the amount of fuels used in different sectors, which could represent the activity levels. It should be noted that the inter-provincial coal transport were not considered in this study. S3

4 63 Table S1. Summary information of solid fuels used in this study Fuel types Stove Sample sites Cities Moisture # of Samples Type (Provinces) content (%) Crop straws Wheat Stove A Shandong Yantai Corn Stove A Shandong Yantai Bean Stove A Heilongjiang Haerbin Rice straw_n Stove A Shandong Linyi Rice straw_s Stove A Hunan Loudi Woods Willow Stove A Shandong Yantai Poplar Stove A Heilongjiang Haerbin Birch Stove A Shandong Yantai Locust Stove A Shandong Yantai Oak Stove A Heilongjiang Haerbin Ashtree Stove A Heilongjiang Haerbin Sophora Stove A Shandong Yantai japonica Gingko Stove A Shandong Yantai Coals Coal_1 Stove B Shanxi Jincheng Coal_2 Stove B Shanxi Yangquan Coal_3 Stove B Inner Mogolia Baotou Coal_4 Stove B Heilongjiang Jixi Coal_5 Stove B Shandong Jining Coal_6 Stove C Guangdong Jiangmen - 2 Note: - denotes not determined S4

5 Table S2 Characteristics of the coals tested in this study Coal ID a JX JC YZ YQ Producing Area Jixi, Heilongjiang province Jincheng, Shanxi province Yanzhou, Shandong province Yangquan, Shanxi province Rank b MVB SA HVB SA Proximate analysis Moisture (M ad, %) Ash (A d, %) Volatile (V daf, %) Fixed carbon (FC ad, %) Ultimate analysis S t, ad % c C ad % H ad % N ad % O ad % a As coal samples from Baotou (BT) and Jiangmen (JM) are not available, they are not tested. b Rank by ASTM standard classification of coal [American Society for Testing and Material, 2004]. HVB is for high-volatile bituminous coal, MVB for medium-volatile bituminous coal, LVB for low-volatile bituminous coal, and SA for semi-anthracite. c S t, ad % refers to air dried basis total sulfur content in general analysis samples, expressed as a percentage by mass, %. S5

6 Table S3 EF LG used for estimating LG emission and the fraction of LG from coal combustion (LG_Coal) to total LG from the residential solid fuel sector (LG_Total). Provinces EF LG (mg kg -1 fuel) LG_Coal Coal Crop Wood BRQ /LG_Total Heilongjiang % Jilin % Liaoning % Neimeng % Hebei % Beijing % Tianjin % Shandong % Henan % Shanxi % Shaanxi % Ningxia % Gansu % Qinghai % Xinjiang % Note: EF LG is the province specific emission factor for different fuels with consideration of the typical fuel types and coal maturity in different provinces. S6

7 Table S4. Ratios with the +/- standard deviation of LG to other water-soluble saccharides measured in solid fuel combustion samples and ambient samples in this study. Ratios Crop straw Wood Coal Ambient samples LG/Arabinose 188± ± ± ±16.9 LG/Galactose 287± ± ± ±37.8 LG/Glucose 81.1± ± ± ±3.62 LG /Mannose 450± ± ± ±51.8 LG /Xylose 65.0± ± ± ±7.78 LG /Glycerol 48.3± ± ± ±1.24 LG /Inositol 122± ± ± ±267 LG /Mannitol 65.5± ± ± ±61.7 LG /Threitol 77.7± ± ± ±68.7 S7

8 Figure S1. Source testing system with combustion equipment and sampling system. (Note: MFC denotes mass flow controller) S8

9 Figure S2. Profiles of saccharides for each type of solid fuel combustion source sample shown as box and whisker plots. Panel A: Crop straw burning samples; Panel B: Wood burning samples; Panel C: Coal combustion samples (Note: Percentage of LG here is shown as one tenth of the real value) S9

10 Figure S3. LG/MN and LG/GA ratios in biomass burning and coal combustion emissions. (Note: Error bars represent one standard deviation) 90 S10

11 References 1. Ma, Q.; Cai, S. Y.; Wang, S. X.; Zhao, B.; Martin, R. V.; Brauer, M.; Cohen, A.; Jiang, J. K.; Zhou, W.; Hao, J. M.; Frostad, J.; Forouzanfar, M. H.; Burnett, R. T. Impacts of coal burning on ambient PM 2.5 pollution in China. Atmos. Chem. Phys. 2017, 17(7), S11