Supporting Information for. Spatiotemporal Trends of Elemental Carbon and Char/Soot Ratios in

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1 Supporting Information for Spatiotemporal Trends of Elemental Carbon and Char/Soot Ratios in Five Sediment Cores from Eastern China Marginal Seas: Indicators of Anthropogenic Activities and Transport Patterns Yin Fang,,,# Yingjun Chen, *,, Tian Lin, *,ǁ Limin Hu,, Chongguo Tian, Yongming Luo, Xin Yang,,ψ Jun Li, # and Gan Zhang # Key Laboratory of Cities Mitigation and Adaptation to Climate Change in Shanghai, College of Environmental Science and Engineering, Tongji University, Shanghai, , China. Shanghai Institute of Pollution Control and Ecological Security, Shanghai, , China. Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai, , China. ǁ State Key Laboratory of Environmental Geochemistry, Guiyang Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, , China. Key Laboratory of Marine Sedimentology and Environmental Geology, First Institute of Oceanography, State Oceanic Administration, Qingdao, , China. Laboratory for Marine Geology, Qingdao National Laboratory for Marine Science S1

2 and Technology, Qingdao, , China. # State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, , China. ψ Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan University, Shanghai, , China *Corresponding authors: College of Environmental Science and Engineering, Tongji University, Shanghai, , China. Phone/fax: ; yjchentj@tongji.edu.cn (Yingjun Chen). State Key Laboratory of Environmental Geochemistry, Guiyang Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, , China. Phone/fax: ; lintian@vip.gyig.ac.cn (Tian Lin) Number of pages: 22 Number of tables: 4 Number of texts: 2 Number of figures: 6 S2

3 41 Table S1. Detailed Descriptions of Five Sediment Cores from the Eastern China Marginal Seas core sampling location latitude, longitude sampling date water depth (m) core length (cm) interval (cm) sedimentation rate (cm yr -1 ) BHS central Bohai Sea N, E August, NYS central northern Yellow Sea N, E June, SYS central southern Yellow Sea N, E June, a ECS1 coastal East China Sea N, E June, ECS2 coastal East China Sea N, E April, or 2 b a The sedimentation rate for core SYS was estimated from previous studies conducted in the southern Yellow Sea region, 1,2 and an approximate value of 0.20 cm yr -1 was used as a reference. b Core ECS2 in the East China Sea was sectioned in 1 cm interval above 100 cm and in 2 cm interval below 100 cm. S3

4 45 46 Table S2. Data of 210 Pb Dating for Sediment Cores BHS, NYS, ECS1, and ECS2 from the Eastern China Marginal Seas 47 depth (cm) core BHS core NYS core ECS1 core ECS2 Pb excess (dpm g -1 ) depth (cm) Pb excess (dpm g -1 ) depth (cm) Pb excess (dpm g -1 ) depth (cm) Pb excess (dpm g -1 ) S4

5 48 49 Table S3. Summary of EC Concentrations in Marine Sediment of NIST SRM-1941b Measured Following IMPROVE TOR Method concentrations (mg g -1 ) number of samples references ± this study ± ± ± ± S5

6 51 52 Table S4. The Geochemical Parameters Measured in Five Sediment Cores from the Eastern China Marginal Seas 53 (1) Core BHS in central mud area from the Bohai Sea grain size (%) concentrations (mg g -1 ) fluxes (g m -2 yr -1 ) ratios (%) year Char/ Soot/ Char/ clay silt sand EC Char Soot EC Char Soot EC EC Soot Min Max Mean SD S6

7 54 (2) Core NYS in central mud area from the northern Yellow Sea 55 grain size (%) concentrations (mg g -1 ) fluxes (g m -2 yr -1 ) ratios (%) year Char/ Soot/ Char/ clay silt sand EC Char Soot EC Char Soot EC EC Soot Min Max Mean SD S7

8 56 (3) Core SYS in central mud area from the southern Yellow Sea 57 grain size (%) concentrations (mg g -1 ) fluxes (g m -2 yr -1 ) ratios (%) year Char/ Soot/ Char/ clay silt sand EC Char Soot EC Char Soot EC EC Soot Min Max Mean SD S8

9 58 (4) Core ECS1 in northern Min-Zhe coastal mud area from the East China Sea grain size (%) concentrations (mg g -1 ) fluxes (g m -2 yr -1 ) ratios (%) year Char/ Soot/ Char/ clay silt sand EC Char Soot EC Char Soot EC EC Soot S9

10 Min Max Mean SD S10

11 60 (5) Core ECS2 in southern Min-Zhe coastal mud area from the East China Sea grain size (%) concentrations (mg g -1 ) fluxes (g m -2 yr -1 ) ratios (%) year Char/ Soot/ Char/ clay silt sand EC Char Soot EC Char Soot EC EC Soot S11

12 Min Max Mean SD S12

13 Text S1. Analytical Procedure for Sediment Grain Size. About 1 g of the sediment sample was pretreated with 10 ml of 30% (v/v) hydrogen peroxide solution to decompose the organic matter. The sample was then dispersed and homogenized using ultra-sonic vibration for 30 s prior to instrumental analysis. Grain size was determined using a laser Particle Size Analyzer (Mastersizer 2000, Malvern Instruments Ltd., UK). The particle sizes were <4 μm for clay, 4 63 μm for silt and >63 μm for sand. The relative error of the duplicate samples was less than 3% (n = 6) Text S2. Analytical Procedure for Sediment Dating. Cores BHS and ECS1 were dated at the Qingdao Institute of Marine Geology and Guangzhou Institute of Geochemistry following the method described by Zhang et al., 7 respectively. The 210 Pb activities were determined by analyzing the radioactivity of the decay product 210 Po by assuming that the two were at equilibrium. The Po was extracted, purified and self-plated onto silver disks. 209 Po was used as the yield monitor and tracer in quantification. Counting was conducted by computerized multi-channel α spectrometry with gold-silicon surface barrier detectors. The relative error for this method was less than 6%. Cores NYS and ECS2 were dated at the East China Normal University and Nanjing Institute of Geography and Limnology following the method described by Wu et al., 8 respectively. Briefly, the 210 Pb and 226 Ra activities were measured using an Ortec HPGe GWL series well-type coaxial low background intrinsic germanium detector. 210 Pb was determined by gamma emissions at 46.5 kev, and 226 Ra by 295 kev and 352 kev gamma rays emitted by the daughter isotope 214 Pb following 3 weeks of storage in sealed containers to allow radioactive S13

14 equilibration. 210 Pb ex was calculated by subtracting 226 Ra activities from the total 210 Pb activities. The relative error for this method was less than 10%. According to the high correlation between the core depths vs. unsupported 210 Pb activity (Figure S2), the average constant sedimentation rates of 0.47, 0.20, 0.98 and 1.05 cm yr -1 for cores BHS, NYS, ECS1 and ECS2, respectively, could be calculated using the constant activity (CA) model, which are in agreement with those previously reported in the same area. 9,10 The data for these cores beyond 100 years are used only as a reference. S14

15 Figure S1. Spatiotemporal trends of sediment grain size distributions in five sediment cores from the eastern China marginal seas. S15

16 Figure S Pb dating of sediment cores BHS, NYS, ECS1, and ECS2 from the eastern China marginal seas. S16

17 96 97 Figure S3. Statistical data on the socioeconomic development indexes in China (National bureau of statistics of China, 2014). S17

18 98 99 Figure S4. EC emission in China from 1976 to 2014 (Data is from Wang et al. 11 ) S18

19 Figure S5. Temporal trends of EC, char, and soot depositional fluxes in five sediment cores from the eastern China marginal seas. S19

20 Figure S6. Correlations between char, soot, and EC depositional fluxes in five sediment cores from the eastern China marginal seas. S20

21 REFERENCES 1. Alexander, C. R.; DeMaster, D.; Nittrouer, C. Sediment accumulation in a modern epicontinental-shelf setting: the Yellow Sea. Mar. Geol. 1991, 98 (1), Wu, Y.; Zhang, J.; Mi, T.; Li, B. Occurrence of n-alkanes and polycyclic aromatic hydrocarbons in the core sediments of the Yellow Sea. Mar. Chem. 2001, 76 (1), Han, Y. M.; Cao, J. J.; An, Z. S.; Chow, J. C.; Watson, J. G.; Jin, Z. D.; Fung, K.; Liu, S. X. Evaluation of the thermal/optical reflectance method for quantification of elemental carbon in sediments. Chemosphere 2007, 69 (4), Cong, Z.; Kang, S.; Gao, S.; Zhang, Y.; Li, Q.; Kawamura, K. Historical trends of atmospheric black carbon on Tibetan Plateau as reconstructed from a 150-year lake sediment record. Environ. Sci. Technol. 2013, 47 (6), Fang, Y.; Chen, Y.; Tian, C.; Lin, T.; Hu, L.; Huang, G.; Tang, J.; Li, J.; Zhang, G. Flux and budget of BC in the continental shelf seas adjacent to Chinese high BC emission source regions. Global Biogeochem. Cycles 2015, 29 (7), Hu, L.; Shi, X.; Bai, Y.; Fang, Y.; Chen, Y.; Qiao, S.; Liu, S.; Yang, G.; Kornkanitnan, N.; Khokiattiwong, S. Distribution, input pathway and mass inventory of black carbon in sediments of the Gulf of Thailand, SE Asia. Estuar. Coast. Shelf. Sci. 2016, 170, Zhang, G.; Parker, A.; House, A.; Mai, B.; Li, X.; Kang, Y.; Wang, Z. Sedimentary records of DDT and HCH in the Pearl River Delta, south China. Environ. Sci. Technol. 2002, 36 (17), Wu, Y.; Wang, S.; Xinhua, H. Chronology of Holocene lacustrine sediments in Co S21

22 Ngoin, central Tibetan Plateau. Sci. China, Ser. D Earth Sci. 2006, 49 (9), Li, F. Y.; Li, X. G.; Song, J. M.; Wang, G. Z.; Cheng, P.; Gao, S. Sediment flux and source in northern Yellow Sea by 210 Pb technique. Chin. J. Oceanol. Limnol. 2006, 24 (3), Huh, C. A.; Su, C. C. Sedimentation dynamics in the East China Sea elucidated from 210 Pb, 137 Cs and 239,240 Pu. Mar. Geol. 1999, 160 (1), Wang, R.; Tao, S.; Wang, W.; Liu, J.; Shen, H.; Shen, G.; Wang, B.; Liu, X.; Li, W.; Huang, Y. Black Carbon Emissions in China from 1949 to Environ. Sci. Technol. 2012, 46 (14), S22

Persistent effects of the Yellow River on the Chinese marginal seas began at least. ~880 ka ago

Persistent effects of the Yellow River on the Chinese marginal seas began at least ~880 ka ago Zhengquan Yao, Xuefa Shi, Shuqing Qiao, Qingsong Liu, Selvaraj Kandasamy, Jianxing Liu, Yanguang Liu, Jihua