Emissions of Halogenated Compounds in East Asia Determined from. Measurements at Jeju Island, Korea

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1 Supporting Information Emissions of Halogenated Compounds in East Asia Determined from Measurements at Jeju Island, Korea Shanlan Li 1,, Jooil Kim 1,, Kyung-Ryul Kim 1,*, Jens Mühle 3, Seung-Kyu Kim 1, Mi-Kyung Park 1,, Andreas Stohl, Dong-Jin Kang 5, Tim Arnold 3, Christina M. Harth 3, Peter K. Salameh 3, and Ray F. Weiss 3 1 School of Earth and Environmental Sciences, Seoul National University, Seoul, South Korea Research Institute of Oceanography, Seoul National University, Seoul, South Korea 3 Scripps Institution of Oceanography, University of California, San Diego, La Jolla, CA, USA Norwegian Institute for Air Research, Kjeller, Norway 5 Korea Ocean Research and Development Institute, Seoul, South Korea *Corresponding author phone: ; fax: The supporting information contains: Text Section 1: Detailed description of source region classification. Table S1: Measurement precisions of halogenated compounds measured at Gosan for year. Table S: Comparisons of emissions derived in this study with other studies for year. Figure S1: Map showing the measurement station at Gosan, Jeju Island, Korea along with the four source regions in this study. Figure S: The residence time analysis using trajectories arriving at Gosan for year. Figure S3: Emissions for year from this study compared with previous studies. Figure S: Relative contributions of emissions from each country within East Asia. 1

2 Text Section 1: Detailed description of source region classification For source region classification we combined air-mass back-trajectory analysis with a tracer method based on the HFC-3/HCFC- ratio. For the back-trajectory analysis, we defined regional grid boxes representing each country in East Asia as shown in Figure S1, and for each -day kinematic back trajectory arriving at Gosan we calculated the residence time following Poirot and Wishiski 1 : n τ ( i, j, a) = S ( i, j, n, a) / V n= 1 ( n, a) τ (i,j,a) is residence time for a th trajectory over grid square (i,j), S (i,j,n,a) is length of that portion of the n th segment of the a th trajectory which falls over grid square (i,j), and V (n,a) is average speed of the air parcel as it travels along the n th segment of the a th trajectory. If a trajectory stayed below the planetary boundary layer (m) for more than 1hour in one of the four regional grid boxes, the air mass was retained in our analysis and classified accordingly. Results of the back trajectory analysis showed that 19% of air-masses affected by mainland China, while %, 19% and % of air-masses affected by Taiwan, Korea, and Japan, respectively. This method was effective in distinguishing the overall influence of the four countries, however many of the trajectories were determined to be of mixed origin (i.e. stayed in two or more regions more than 1hour), most notably mixes of Chinese and Korean influence (which accounted for 3% of all measurements). To further analyze these mixes from China and Korea, the HFC-3/HCFC- ratio was used as a tracer to determine the influence from China. China is a dominant source of HFC-3 emissions in East Asia, due to industrial production of HCFC-. In contrast, Korea has participated in Clean Development Mechanism (CDM) projects to incinerate HFC-3 emission from industrial production of HCFC-. 3 The HFC-3/HCFC- ratios for air-masses originating from China

3 (.1) are higher than those from other regions (below.). Therefore, China/Korea mixed events with HFC-3/HCFC- ratio higher than.1 (~15% of China/Korea mixed events) were also discussed as influenced from China together with air-masses classified by back- trajectory analysis (~19%). 3

4 Reference (1) Poirot, R.L.; Wishinski, P. R. Visibility, sulfate and air mass history associated with the summertime aerosol in Northern Vermont. Atmos. Environ., 19, (7), () Kim, J.; Li, S.; Kim, K.R.; Stohl, A.; Mühle, J.; Kim, S.K.; Park, M.K.; Kang, D.J.; Lee, G.; Harth, C.M.; Salameh, P.K.; Weiss, R.F. Regional atmospheric emissions determined from measurements at Jeju Island, Korea: Halogenated compounds from China, Geophys. Res. Lett. 1, 37, L11. (3) CDM () Clean Development Mechanism: HFC-3 decomposition project in Ulsan. (available at cdm.unfcc.int/projects/db/jqa /view). () Li, S.; Kim, J.; Kim, K.R.; Mühle, J. Emission characteristics of HFC-3 (CHF3)/HCFC- (CHClF) between different air masses in Notheastern Asia, J. Kor. Soci. Atmos. Environ. 1, (5), 9-9. (In Korean).

5 Table S1: Measurement precisions halogenated compounds measured at Gosan for year annual mean standard Compounds precision (%RSD) CFC-11.1 CFC-1. CFC-113. CFC-11.1 HCFC-.1 HCFC-11b.51 HCFC-1b.9 HFC-3. HFC-13a.3 HFC-15a. HFC-3 1. HFC-15. HFC-13a.73 HFC-35mfc 3.7 H CF.1 C F.59 C 3 F 1. SF.3 CH 3 Cl.15 CH Cl.3 CHCl 3.3 CH 3 CCl 3. CH 3 Br. 5

6 Table S. Comparisons of emissions derived in this study for Nov. 7 to Dec. with Stohl et al. (1) for year and Saito et al. (1) for Nov. 7 to Sep. 9. China mainland Taiwan region Korea Japan Compounds This Study Stohl et al.(1) This Study Stohl et al.(1) This Study Stohl et al.(1) This study Stohl et al.(1) HCFC- 3 (-19).1 ±..1 ±.5. ±.5. (-.) 7.9 ± (1-13) 5.9 ±.3 HCFC-11b 15 (11-1) 1 ±1.5.5 ±.11.5 ±.1. (.-.5) 1.9 ±.3 1. (1.-.) 1.1 ±.1 HCFC-1b 9 (.9-13) 7.7 ±.7.1 ±.3.3 ±.1. (.7-.9). ±.1.9 (.7-1.). ±.1 HFC-3 1 (7.-13).1 ±..7 ±..3 ±.1.11 (.-.13). ±.5.3 (.-.3). ±.1 HFC-13a.3 (.-11) 11. ±1.7.5 ±.1. ±. 1.7 (1.5-1.) 1. ±.3.7 (.5-5) 3.1 ±. HFC-15a 5. (.-7.) 3. ±.5. ±.. ±.1.11 (.-.13).1 ±. 1. (1.1-1.). ±.1 This Study Saito et al.(1) This Study Saito et al. (1) This Study Saito et al. (1) This study Saito et al. (1) C F.5 (.-.7).99 ±.3.1 (.9-.1).9 ±.. (.1-.).19 ±.1 C 3 F.9 (.-.13).157 ±.3. (.3-.).31 ±..91 ±.19

7 Figure S. The residence time analysis using -day back-trajectories arriving at Gosan for year. 7

8 CFCs [ODP-kt] China HCFCs [ODP-kt] 1 1 China CFCs [ODP-kt] 1 Korea HCFCs [ODP-kt] 1 Korea CFCs [ODP-kt] 1 Japan HCFCs [ODP-kt] 1 Japan Time Time Figure S3. Emissions for year from this study (red) compared to emission estimates from Palmer et al. [3] (green), Yokouchi et al. [5] (purple, only HCFC-), Yokouchi et al. [] (pink), Stohl et al. [9] (cyan, only HCFC-), Vollmer et al. [9] (dark green, HCFC- and HCFC-1b), Wan et al. [9] (dark blue) and consumption data reported to UNEP (blue).

9 Percentage to East Asian emission (%) 1 China Taiwan Korea Japan CFC-11 CFC-1 CFC-113 CFC-11 HCFC- HCFC-11b HCFC-1b HFC-3 HFC-13a HFC-15a HFC-3 HFC-15 HFC-13a HFC-35mfc H-111 CF C F C 3 F SF CH 3 Cl CH Cl CHCl 3 CH 3 CCl 3 CH 3 Br Figure S. Relative contributions of emissions from each country within East Asia. 9