Supporting Information

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1 1 Supporting Information MANUSCRIPT TITLE: AUTHORS: ADDRESS: Sediment Records of Polycyclic Aromatic Hydrocarbons (PAHs) in the Continental Shelf of China: Implications for Evolving Anthropogenic Impacts Liang-Ying Liu, Ji-Zhong Wang, Gao-Ling Wei, Yu-Feng Guan, Charles S. Wong, and Eddy Y. Zeng State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 5164, China, Environmental Studies Program and Department of Chemistry, Richardson College for the Environment, University of Winnipeg, Winnipeg, Manitoba, R3B 2E9 Canada and Graduate School of Chinese Academy of Sciences, Beijing 149, China FIGURES: 11 TABLES: 1 NO. OF PAGES: 14 S1

2 Table 1. Descriptions of sediment cores from Yellow Sea (YS) and South China Sea (SCS), and summary of Σ 15 PAH concentration ranges within each entire core Core sedimentation focusing Water Core Diameter Concentration rate (cm yr -1 ) factor depth (m) length (cm) (cm) range (ng g -1 ) YS1.3 a / Y S1.2 b a 21 Pb activity in core YS1 was not analyzed; this rate was a result deduced from previous studies. 22,26 b If the 21 Pb data in an increment in the deeper layer was removed, the sedimentation rate in this core would become.6 cm yr -1. Sediment focusing factors in cores Y and were fitted with a three-parameter exponential decay model, 29 while that in core S1 was fitted with a two-parameter exponential decay model.

3 total consumption (a) Energy Consumption (1 8 tons) Shandong Shanxi Hebei Jiangsu Guangdong (b) Figure S1. (a) Historical profiles of total energy consumption in China and (b) coal consumption in selected coastal provinces in North China (Shandong, Shanxi, Hebei and Jiangsu Provinces; Figure 1) and South China (Guangdong Province; Figure 1). Data were compiled from Statistics data on 6 years of new China. 1 The unit is 1 8 tons standard coal. S3

4 Depth (cm) Y S1 5 Y= -7.7 Ln(x) R 2 =.62 Y= Ln(x) R 2 = Y= Ln(x) R 2 = Ln ( 21 Pb excess ) Figure. 21 Pb age dating of sediment cores Y, S1, and in the coastal marine systems off China. Average sedimentation rate is.3,.2, and.5 cm yr -1 in Y, S1, and, respectively. If the symbol embodied in dark-line ellipse was excluded, the sedimentation rate in core S1 would become.6 cm yr -1. S4

5 1 1 Depth (cm) YS1 Y S Y S Concentrations (ng g -1 ) FF-corrected Concentrations (ng g -1 ) Figure S3. Depth profiles of focusing factor (FF)-corrected and non-corrected Σ 15 PAH concentrations in sediment cores from Yellow Sea and the SCS. Σ 15 PAH is the sum of acenapthylene, acenaphthane, fluorene, phenanthrene, anthracene, fluoranthene, pyrene, benzo[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene, indeno[1,2,3-cd]pyrene, didenzo[a,h]anthracene, and benzo[g,h,i]perylene. S5

6 YS Y S Relative Abundance Figure S4. Depth profiles of the percentages of 2+3-ring (the sum of Acy, Ace, Flo, Phe, and An; left), 4-ring (the sum of Fl, Py, BaA and Chr; middle), and 5+6-rings (the sum of BbF, BkF, BaP, IcdP, DahA, and BghiP; right) PAHs to Σ 15 PAH (16 USEPA priority pollutants minus naphthalene) in coastal marine sediment cores off China. S6

7 Phe Py Fl BaA Chr BaP 4 8 BbF IcdP BghiP Per YS Concentration (ng g -1 ) Figure S5. Historical trends of individual PAH concentrations (ng g -1 dry weight) in sediment cores from the Yellow Sea (YS1) and the South China Sea (). Upward arrows indicate up ticks and downward arrows suggest bottom ticks. Concentrations for core was focusing factor (5.6; SI Table S1) corrected. S7

8 1 1 Depth (cm) YS1 Y S Fl/(Fl+Py) Depth (cm) YS1 Y S IcdP/(IcdP+BghiP) Figure S6. Depth profile of source diagnostic ratios, Fl/(Fl+Py) and IcdP/(IcdP+BghiP) in coastal marine sediment cores from Yellow Sea and the SCS. Fl, Py, IcdP, and BghiP are the abbreviations for fluoranthene, pyrene, indeno[1,2,3- cd]pyrene, and benzo[g,h,i]perylene, respectively. S8

9 (a) (b) Relative Distribution 1. Y S Figure S7. acenaphthylene acenaphthene fluorene phenanthrene anthracene fluoranthene pyrene benzo(a)anthracene chrysene benzo(b)fluoranthene benzo(k)fluoranthene benzo(a)pyrene dibenzo(a,h)anthracene iden(123-cd)pyrene benzo(ghi)perylene straw wood coal briquette acenaphthylene acenaphthene fluorene phenanthrene anthracene fluoranthene pyrene benzo(a)anthracene chrysene benzo(b)fluoranthene benzo(k)fluoranthene benzo(a)pyrene dibenzo(a,h)anthracene iden(123-cd)pyrene benzo(ghi)perylene Comparison of PAH compositions in marine sediments with emission profiles from coal (e.g., coal briquette) and biomass (e.g., straw and wood). Individual PAH compound in sediment cores (average of the entire core) was normalized to benzo[b]fluoranthene (a) and those in typical combustion sources were normalized to phenanthrene (b). S9

10 Acy Ace Flo Phe An Annual Emission Rates in China (tons) Fl Py BaA Chr BbF BkF BaP DahA BghiP IcdP straw firewood domestic coal coking industry industrial coal transport petroleum Emission Sources other petroleum aluminum production Figure S8. Annual emission rates (tons) of PAH compounds from typical combustion sources in China in 23. Data was compiled from a published study. 2 S1

11 Gross Domestic Production (1 billion Yuan) Figure S9. Historical changes in Chinese gross domestic production. Data were obtained from Statistics data on 6 years of new China. 1 S11

12 Coal Petroleum Coal% (a) (b) Energy Consumption (1 7 tons) Figure S1. (a) Historical Chinese consumption of petroleum; (b) historical consumption of coal and the percent contribution of coal to total energy consumption. Data were compiled from Statistics data on 6 years of new China. 1 The unit is 1 7 tons standard coal. S12

13 Coal coal natural gas liquefied petroleum gas Natural Gas and Liquefied Petroleum Gas Figure S11. Historical changes in annual average household consumption of major energy sources (coal, natural gas and liquefied petroleum gas) in China. Data were compiled from Statistics data on 6 years of new China. 1 The unit for coal and liquefied petroleum gas is kilogram (kg), and cubic meter (m 3 ) for natural gas. S13

14 REFERENCES (1) National Bureau of Statistics of China Statistics data on 6 years of new China (in Chinese); China Statistics Press: Beijing, 28. (2) Xu, S. S.; Liu, W. X.; Tao, S. Emission of polycyclic aromatic hydrocarbons in China. Environ. Sci. Technol. 26, 4, S14