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Supplementary material

Characteristic concentrations and isotopic composition of airborne lead at

urban, rural and remote sites in western Korea

Sanghee Lee1,2, Daechol Shin1, Changhee Han3, Kwang-Sik Choi4, Soon Do Hur3, Jooyoung

Lee5, Do-Seong Byun5, Young-Taeg Kim5, Sungmin Hong1,*

1Department of Ocean Sciences, Inha University, 100 Inha-ro, Michuhol-gu, Incheon 22212, Korea2National Institute of Environmental Research, Hwangyong-ro 42, Seogu, Incheon 22689, Korea3Korea Polar Research Institute, 26 Songdomirae-ro, Yeonsu-gu, Incheon 21990, Korea4School of Marine Biomedical Science (BK21 PLUS), Jeju National University, 102 Jejudaehak-ro, Jeju-si, Jeju Special Self-Governing Province, 63243, Korea5Korea Hydrographic and Oceanographic Agency, 351, Haeyang-ro, Yeongdo-gu, Busan 49111, Korea

*Corresponding author: Email: [email protected] (Sungmin Hong); Phone: +82-32-860-

7708; Fax: +82-32-862-5236

Summary

There are 13 pages in this Supplementary Material including 6 figures and 3 tables.

SI Figure 1. Three-isotope plots of 206Pb/207Pb vs. 208Pb/207Pb during the individual seasons at 1

IC, TA, and JJ. Also included are the ranges in isotopic compositions of atmospheric Pb for China, Korea, Japan, and Taiwan from the literature. A filled square represents the Pb isotopic composition of airborne Pb collected in a road tunnel (see text).

SI Figure 2. The Pb isotopic compositions in aerosols collected at various sites in Korea (Fig. 1). (a) The Korean Pb isotopic field previously reported by Lee et al. (2017). Deleted data in

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Table S2 of the supplementary material are shown in red color. (b) The Korean Pb isotopic field modified by using the data listed in Table S2. New data added to a database table, Table S2, are shown in blue color.

SI Figure 3. Examples of the HYSPLIT back trajectories for samples listed in Table S2 of the supplementary material. Colored lines represent the mean trajectory of each cluster. Four

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main trajectory clusters are numbered and values in parentheses are the percentage of backward air trajectories included in each cluster. (a, b) The air masses arriving at Cheonan (CA) and Geochang (GC) during the sampling periods. They were transported over Korea and thus referred to as the local air masses. The isotopic compositions of the samples characterized by the local air masses were used for the determination of the Pb isotopic field for Korean aerosols (SI Fig. 2). (c, d) The air masses of Yeosu 1 (YS1) and Ulsan (US) represented trajectories originating dominantly from regions outside Korea. The isotopic compositions of the samples associated with such air mass pathways were excluded from the Korean Pb isotopic field (see Table S2).

SI Figure 4. Representative results of the HYSPLIT model 5-day backward trajectory analysis of the Asian Dust periods observed at IC, TA and JJ. Numbers denote the sample

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numbers shown in Fig. 4 (see text).

SI Figure 5. Results of the HYSPLIT model 3-day backward trajectory analysis for the samples showing 208Pb-depleted isotopic composition at JJ. Numbers denote the sample

5

numbers shown in Fig. 4 (see text).

SI Figure 6. Location map of the major domestic sources (coal power plants, iron and steel works, non-ferrous metal smelters, and petrochemical industrial complexes) situated in southeastern Korea.

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Table S1. Al and Pb concentrations, enrichment factors for Pb, and Pb isotope ratios determined in 141 TSP samples collected at urban (IC), rural (TA), and remote (JJ) sites.

Sample Sampling period(dd/mm/yy)

Duration(h)

Concentration (ng m–3) Enrichmentfactor

Pb isotope ratio Inferred major source regionAl Pb 206Pb/207Pb 208Pb/207Pb

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IC 1 31/08/15-10/09/15 230 h 651 18.6 130 1.159 2.431 KoreaIC 2 10/09/15-17/09/15 168 h 950 23.5 113 1.154 2.438 China/KoreaIC 3 17/09/15-24/09/15 172 h 1521 49.4 148 1.156 2.431 KoreaIC 4 24/09/15-01/10/15 168 h 1679 25.6 70 1.133 2.429 KoreaIC 5 12/10/15-19/10/15 161 h 537 4.76 40 1.158 2.433 ChinaIC 6 19/10/15-26/10/15 164.5 h 1222 10.2 38 1.153 2.434 China/KoreaIC 7 26/10/15-02/11/15 168 h 895 5.42 28 1.164 2.435 ChinaIC 8 09/11/15-16/11/15 169 h 563 6.52 53 1.152 2.442 KoreaIC 9 16/11/15-23/11/15 170.5 h 596 8.47 65 1.137 2.425 Korea

IC 10 23/11/15-30/11/15 165.5 h 510 12.5 112 1.159 2.439 China/KoreaIC 11 30/11/15-07/12/15 167 h 719 10.9 69 1.160 2.438 ChinaIC 12 07/12/15-14/12/15 173 h 1736 49.8 131 1.161 2.440 ChinaIC 13 14/12/15-24/12/15 236.5 h 925 16.8 83 1.160 2.444 ChinaIC 14 24/12/15-31/12/15 167 h 700 16.8 110 1.155 2.436 ChinaIC 15 31/12/15-07/01/15 169 h 591 14.9 115 1.158 2.438 ChinaIC 16 07/01/15-14/01/16 170.5 h 974 27.8 130 1.157 2.441 ChinaIC 17 14/01/16-21/01/16 168 h 451 5.23 53 1.154 2.438 China/KoreaIC 18 21/01/16-28/01/16 169.5 h 2023 43.7 98 1.159 2.443 ChinaIC 19 28/01/16-04/02/16 168 h 1726 49.9 132 1.159 2.445 ChinaIC 20 04/02/16-11/02/16 169 h 1826 54.2 135 1.159 2.444 ChinaIC 21 11/02/16-18/02/16 169 h 754 16.8 101 1.162 2.441 ChinaIC 22 18/02/16-25/02/16 166 h 2012 39.4 89 1.157 2.440 ChinaIC 23 25/02/16-04/03/16 185 h 1164 21.3 83 1.158 2.434 ChinaIC 24 04/03/16-10/03/16 152 h 2450 17.7 33 1.155 2.440 China/KoreaIC 25 10/03/16-19/03/16 211 h 1481 30.1 93 1.160 2.439 ChinaIC 26 19/03/16-24/03/16 125 h 1289 21.0 74 1.153 2.433 ChinaIC 27 24/03/16-31/03/16 168 h 1535 19.5 58 1.157 2.441 ChinaIC 28 31/03/16-07/04/16 167 h 1251 12.4 45 1.154 2.431 ChinaIC 29 07/04/16-14/04/16 168.5 h 580 4.84 38 1.154 2.441 China/KoreaIC 30 14/04/16-21/04/16 168 h 962 11.9 57 1.153 2.430 China/KoreaIC 31 21/04/16-28/04/16 168 h 2319 11.4 22 1.156 2.438 China/KoreaIC 32 28/04/16-12/05/16 167.5 h 2086 22.8 50 1.148 2.434 China/KoreaIC 33 12/05/16-19/05/16 172 h 809 16.9 95 1.159 2.441 ChinaIC 34 19/05/16-26/05/16 165 h 972 13.8 65 1.155 2.438 KoreaIC 35 26/05/16-02/06/16 170 h 1121 12.0 49 1.152 2.444 ChinaIC 36 02/06/16-09/06/16 166 h 355 3.00 38 1.150 2.432 KoreaIC 37 09/06/16-16/06/16 166 h 446 6.15 63 1.154 2.430 KoreaIC 38 16/06/16-23/06/16 172 h 279 3.17 52 1.150 2.434 KoreaIC 39 23/06/16-30/06/16 166 h 401 8.69 99 1.154 2.430 China/KoreaIC 40 30/06/16-07/07/16 168 h 113 2.06 84 1.151 2.431 China/Korea


Duration(h)



IC 41 07/07/16-14/07/16 169 h 298 4.52 69 1.145 2.436 KoreaIC 42 14/07/16-21/07/16 168 h 185 1.92 47 1.141 2.432 KoreaIC 43 21/07/16-28/07/16 169 h 300 2.07 32 1.153 2.435 Korea/JapanIC 44 28/07/16-04/08/16 169 h 262 4.03 70 1.143 2.427 Korea

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IC 45 04/08/16-25/08/16 503 h 538 5.81 49 1.135 2.432 KoreaIC 46 25/08/16-01/09/16 168 h 276 2.98 49 1.149 2.437 China/KoreaIC 47 01/09/16-08/09/16 168 h 183 2.39 60 1.152 2.435 China/KoreaIC 48 08/09/16-27/09/16 451 h 216 3.59 76 1.144 2.430 KoreaIC 49 27/09/16-06/10/16 221.5 h 723 16.3 103 1.146 2.436 China/KoreaTA 1 05/09/15-12/09/15 171.5 h 707 16.0 103 1.158 2.430 KoreaTA 2 12/09/15-19/09/15 160 h 703 15.1 98 1.161 2.428 KoreaTA 3 19/09/15-25/09/15 148 h 63.2 0.274 20 1.159 2.437 China/KoreaTA 4 25/09/15-06/10/15 263 h 1224 24.8 92 1.149 2.444 ChinaTA 5 06/10/15-13/10/15 166.5 h 1089 20.0 84 1.156 2.438 ChinaTA 6 13/10/15-20/10/15 176.5 h 375 6.98 85 1.161 2.440 ChinaTA 7 20/10/15-27/10/15 160.5 h 507 7.21 65 1.156 2.440 ChinaTA 8 10/11/15-17/11/15 168 h 106 3.65 156 1.142 2.429 KoreaTA 9 17/11/15-24/11/15 168 h 71.1 1.44 92 1.161 2.441 China

TA 10 24/11/15-02/12/15 192 h 94.9 3.77 181 1.163 2.434 ChinaTA 11 02/12/15-09/12/15 168 h 802 4.30 24 1.155 2.438 ChinaTA 12 09/12/15-14/12/15 123 h 476 9.30 89 1.151 2.439 China/KoreaTA 13 14/12/15-23/12/15 216 h 444 24.9 255 1.159 2.437 China/KoreaTA 14 23/12/15-31/12/15 198.5 h 402 6.13 69 1.149 2.445 ChinaTA 15 31/12/15-19/01/16 456 h 471 23.1 223 1.160 2.441 ChinaTA 16 19/01/16-27/01/16 192 h 887 9.51 49 1.152 2.438 ChinaTA 17 27/01/16-02/02/16 144 h 447 9.94 101 1.149 2.441 ChinaTA 18 02/02/16-10/02/16 192 h 907 10.7 54 1.152 2.439 ChinaTA 19 10/02/16-17/02/16 168 h 904 13.6 69 1.158 2.442 ChinaTA 20 17/02/16-24/02/16 168 h 917 12.4 62 1.156 2.434 ChinaTA 21 24/02/16-02/03/16 168 h 894 17.8 90 1.159 2.443 ChinaTA 22 02/03/16-09/03/16 168 h 3123 21.8 32 1.152 2.467 ChinaTA 23 16/03/16-23/03/16 168 h 1069 43.1 184 1.148 2.430 ChinaTA 24 23/03/16-30/03/16 171 h 535 10.3 88 1.155 2.439 ChinaTA 25 30/03/16-06/04/16 168 h 822 6.05 34 1.153 2.438 ChinaTA 26 06/04/16-13/04/16 168 h 1021 5.48 24 1.151 2.440 ChinaTA 27 13/04/16-20/04/16 168 h 847 17.4 94 1.156 2.438 ChinaTA 28 20/04/16-27/04/16 168 h 2402 12.1 23 1.150 2.442 ChinaTA 29 27/04/16-04/05/16 168 h 752 8.56 52 1.141 2.440 ChinaTA 30 04/05/16-11/05/16 168 h 2136 21.6 46 1.158 2.449 ChinaTA 31 11/05/16-18/05/16 168 h 637 9.17 66 1.155 2.433 ChinaTA 32 18/05/16-25/05/16 168 h 780 9.00 53 1.154 2.437 China/KoreaTA 33 25/05/16-01/06/16 168 h 865 8.04 42 1.157 2.444 ChinaTA 34 01/06/16-08/06/16 168 h 770 10.0 59 1.141 2.439 China/Korea


Duration(h)



TA 35 08/06/16-15/06/16 168 h 337 9.71 131 1.158 2.443 ChinaTA 36 15/06/16-22/06/16 168 h 363 14.4 180 1.166 2.441 ChinaTA 37 22/06/16-29/06/16 168 h 475 19.8 190 1.159 2.430 KoreaTA 38 29/06/16-06/07/16 168 h 138 4.77 157 1.164 2.440 ChinaTA 39 06/07/16-13/07/16 168 h 347 6.02 79 1.143 2.430 Korea

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TA 40 13/07/16-20/07/16 168 h 177 2.14 55 1.154 2.434 KoreaTA 41 20/07/16-27/07/16 168 h 109 3.19 133 1.158 2.429 KoreaTA 42 27/07/16-03/08/16 168 h 168 3.14 85 1.156 2.441 ChinaTA 43 03/08/16-10/08/16 168 h 637 14.2 101 1.127 2.439 KoreaTA 44 10/08/16-17/08/16 168 h 232 2.94 58 1.143 2.440 China/KoreaTA 45 17/08/16-24/08/16 168 h 547 11.5 95 1.139 2.432 KoreaTA 46 24/08/16-31/08/16 168 h 15.1 0.669 201 1.151 2.434 China/KoreaTA 47 31/08/16-07/09/16 168 h 397 8.51 98 1.156 2.440 China/KoreaTA 48 07/09/16-13/09/16 168 h 154 4.24 125 1.156 2.437 ChinaTA 49 13/09/16-20/09/16 168 h 218 4.66 97 1.152 2.441 China/KoreaTA 50 20/09/16-27/09/16 168 h 618 21.6 159 1.148 2.436 China/KoreaTA 51 27/09/16-04/10/16 168 h 255 11.7 209 1.146 2.434 China/Korea

JJ 1 01/09/15-08/09/15 162 h 233 4.79 94 1.163 2.436 KoreaJJ 2 08/09/15-15/09/15 172 h 342 4.80 64 1.156 2.429 KoreaJJ 3 15/09/15-22/09/15 164 h 488 10.5 98 1.146 2.431 KoreaJJ 4 22/09/15-30/09/15 192 h 62.1 2.80 206 1.154 2.419 KoreaJJ 5 08/10/15-15/10/15 164.5 h 583 5.57 44 1.163 2.437 ChinaJJ 6 15/10/15-23/10/15 189 h 1112 17.9 73 1.151 2.437 KoreaJJ 7 23/10/15-30/10/15 168 h 1000 11.2 51 1.158 2.441 ChinaJJ 8 23/11/15-30/11/15 173 h 192 3.61 86 1.160 2.433 China/KoreaJJ 9 30/11/15-09/12/15 213 h 125 1.75 64 1.159 2.439 China

JJ 10 23/12/15-30/12/15 168 h 220 5.78 120 1.163 2.436 ChinaJJ 11 30/12/15-06/01/16 168 h 104 3.87 169 1.156 2.429 ChinaJJ 12 06/01/16-13/01/16 169 h 56.9 2.51 201 1.146 2.431 ChinaJJ 13 13/01/16-20/01/16 169 h 140 10.8 350 1.154 2.419 ChinaJJ 14 20/01/16-27/01/16 168 h 21.2 0.826 178 1.163 2.437 ChinaJJ 15 27/01/16-03/02/16 168 h 30.4 1.39 208 1.151 2.437 ChinaJJ 16 03/02/16-12/02/16 216 h 206 6.63 146 1.158 2.441 ChinaJJ 17 12/02/16-18/02/16 144 h 103 5.94 263 1.160 2.433 ChinaJJ 18 18/02/16-25/02/16 168 h 361 7.10 90 1.159 2.439 ChinaJJ 19 03/03/16-10/03/16 168 h 9.70 0.895 420 1.151 2.433 KoreaJJ 20 10/03/16-18/03/16 192 h 690 7.35 49 1.161 2.441 China/KoreaJJ 21 18/03/16-30/03/16 288 h 330 1.87 26 1.162 2.437 ChinaJJ 22 30/03/16-04/04/16 120 h 1402 32.2 104 1.163 2.447 ChinaJJ 23 04/04/16-11/04/16 168 h 445 6.19 63 1.156 2.440 China/KoreaJJ 24 11/04/16-18/04/16 168 h 2018 15.7 35 1.162 2.435 ChinaJJ 25 18/04/16-25/04/16 168 h 1180 20.2 78 1.159 2.443 ChinaJJ 26 12/05/16-23/05/16 260 h 733 4.81 30 1.155 2.441 China/Korea


Duration(h)



JJ 27 23/05/16-30/05/16 171 h 750 15.7 95 1.162 2.438 ChinaJJ 28 30/05/16-07/06/16 192 h 717 7.81 50 1.146 2.417 KoreaJJ 29 07/06/16-14/06/16 168 h 670 5.00 34 1.163 2.436 Korea/JapanJJ 30 14/06/16-21/06/16 168 h 680 8.72 58 1.162 2.443 China/South AsiaJJ 31 21/06/16-28/06/16 168 h 171 1.84 49 1.164 2.443 ChinaJJ 32 28/06/16-05/07/16 168 h 110 2.16 89 1.150 2.437 China

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JJ 33 05/07/16-12/07/16 168 h 166 1.08 30 1.151 2.432 South AsiaJJ 34 12/07/16-26/07/16 336 h 177 1.37 35 1.167 2.448 China/KoreaJJ 35 26/07/16-17/08/16 504 h 154 0.764 23 1.158 2.438 JapanJJ 36 17/08/16-23/08/16 144 h 478 4.36 42 1.162 2.447 KoreaJJ 37 23/08/16-30/08/16 168 h 366 3.84 48 1.153 2.438 KoreaJJ 38 30/08/16-08/09/16 216 h 445 7.51 77 1.155 2.438 ChinaJJ 39 08/09/16-20/09/16 288 h 106 2.56 110 1.163 2.433 KoreaJJ 40 20/09/16-27/09/16 168 h 11.2 2.33 949 1.161 2.441 KoreaJJ 41 27/09/16-04/10/16 168 h 27.2 0.682 114 1.154 2.433 Korea

Table S2. Pb concentrations and Pb isotope ratios in 29 TSP samples collected at various sites in Korea (Lee et al., 2017). The sampling sites are shown in Fig. 1. When the HYSPLIT cluster analysis indicated that the air masses originated dominantly from regions outside Korea during the sampling period (see SI Fig. 3), the corresponding data were then deleted from the previously reported data set. The supplementary data obtained from this study is referred to as the ‘added’ samples in the table. The Pb isotopic field for Korean aerosols was modified by using the data presented in this table (see text and SI Fig. 2).

Sampling site Sampling period Duratio Pb Pb isotope ratio Note

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n(dd/mm/yy) (hour) (ng m–3) 206Pb/207Pb 208Pb/207Pb

Bucheon (BC) 08/09/15-10/09/15 49 h 17.4 1.157 2.431Busan (BS) 15/08/15-16/08/15 30 h 31.3 1.146 2.419

Cheonan (CA) 05/08/16-06/08/16 21 h 22.1 1.123 2.426

Daejeon 1 (DJ1) 18/09/15-25/09/15 142.5 h 23.7 1.152 2.438

Daejeon 2 (DJ2) 19/06/16-25/06/16 146.5 h 6.22 1.163 2.431

Gangreung (GR) 04/09/15-05/09/15 21 h 4.78 1.147 2.434

Geochang (GC) 13/10/16-15/10/16 44 h 25.7 1.160 2.436 added

Gunsan (GS) 08/09/16-10/09/16 41 h 16.7 1.162 2.443 deleted

Gwanghyewon 1 (GHW1) 21/09/15-25/09/15 90 h 9.63 1.136 2.423

Gwanghyewon 2 (GHW2) 06/09/16-13/09/16 168 h 24.5 1.151 2.442

Gwanghyewon 3 (GHW3) 13/09/16-20/09/16 168 h 2.11 1.147 2.425 added

Jeonju (JEON) 30/06/16-01/07/16 19.5 h 1.96 1.150 2.427 deleted

Jinju (JIN) 03/09/16-12/09/16 201 h 1.81 1.158 2.435

Mokpo (MP) 11/08/16-13/08/16 43 h 8.15 1.136 2.428

Pohang (PH) 13/09/15-17/09/15 98.5 h 5.41 1.149 2.438

Seoul 1 (SU1) 12/08/15-16/08/15 91 h 36.1 1.155 2.432

Seoul 2 (SU2) 25/09/15-02/10/15 172 h 16.4 1.138 2.430 deleted

Seoul 3 (SU3) 28/06/16-11/07/16 79 h 51.5 1.149 2.436

Suwon (SW) 27/08/15-01/09/15 120 h 25.2 1.157 2.437

Uljin (UJ) 13/06/16-17/06/16 95 h 3.43 1.14 2.421

Ulsan (US) 14/07/16-15/07/16 22 h 23.5 1.175 2.445 deleted

Yecheon (YC) 03/08/16-05/08/16 40.5 h 2.97 1.12 2.423

Yeosu 1 (YS1) 31/07/15-03/08/15 72 h 1.92 1.148 2.426 deleted

Yeosu 2 (YS2) 07/08/15-10/08/15 73.5 h 5.22 1.154 2.431

Yeosu 3 (YS3) 17/08/15-21/08/15 97 h 3.12 1.154 2.427

Yeosu 4 (YS4) 10/08/15-17/08/15 159.5 h N/A 1.153 2.431 added

Yeosu 5 (YS5) 21/08/15-24/08/15 79 h N/A 1.144 2.410 added



N/A: Pb concentration was not analyzed.

Table S3. Literature data on the Pb isotope ratios of the potential domestic sources.

Samples 206Pb/207Pb 208Pb/207Pb ReferenceIron/metal industrial complex (IMIC)a Lee et al. (2011)

Furnace dustb 1.1727–1.2026 2.3105–2.3470Airborne Pb from the stackc 1.2026 2.5431

Major importing iron oresOres from Brazil 1.1317–1.1535 2.3332–2.3479 Galarza et al. (2008)

Ores from Australia 0.9280–1.0551 2.2533–2.3275 Brown et al. (2003)Flue gas from domestic non-ferrous Park et al. (2013)

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smeltersZinc smelter 1.105–1.149 ~2.38–2.44Lead smelter 1.136–1.155 ~2.42–2.44

Copper smelter 1.182–1.184 ~2.46Crude oilsd 0.9869–1.2296 2.0549–2.4890 Fetter et al. (2019)Tunnel air samplese 1.1299 2.4251 Lee et al. (2011)Cenozoic basalts in Jeju Island 1.1929–1.2209 2.4982–2.5371 Park et al. (2005)aAn iron and metal industrial complex (IMIC) in Pohang consisting of Pohang Iron and Steel Co. Ltd. (POSCO), the world’s fifth-largest steelmaker operating two steel mills in Pohang and Gwangyang (SI Fig. 6), and numerous iron and steel ferroalloy manufacturing companies.bElectronic arc furnace dust sample at a ferroalloy manufacturing factory within the IMIC.cAir samples from a smelting furnace stack of POSCO.dIsotopic data from 41 crude oil samples originated from distinct locations and environments.eAir samples collected in the middle of a road tunnel.

References:

Brown S.M., Johnson C.A., Watling R.J., Premo W.R., Constraints on the composition of ore fluids and implications for mineralizing events at the Cleo gold deposit, Eastern Goldfields Province, Western Australia Aust. J. Earth Sci. 50, 2003, 19–38.

Fetter N., Blichert-Toft J., TéloukP., AlbarèdeF., Extraction of Pb and Zn from crude oil for high-precision isotopic analysis by MC-ICP-MS, Chem. Geol., 511, 2019, 112–122.

Galarza M.A., Macambira M.J.B., Villas R.N., Dating and isotopic characteristics (Pb and S) of the Fe oxide-Cu-Au-U-REE Igarapé Bahia ore deposit, Carajás mineral Province, Pará state, Brazil, J. South Am. Earth Sci., 25, 2008, 377–397.

Park K.H., Park J.B., Cheong C.S., Oh C.W., Sr, Nd and Pb isotopic systematics of the Cenozoic basalts of the Korean Peninsula and their implications for the Permian-Triassic continental collision boundary Gondwana Res., 8, 2005, 529-538

Park J.-J., Kim K.-J., Park J.-S., Yoo S.-M., Park K.-S., Seok K.-S., Shin H.-S., Song G.-J., Kim Y.-H., Characterization of lead isotope emission profiles in non-ferrous smelters in South Korea, Anal. Sci. Technol., 26 (5), 2013, 333-339, (in Korean with English abst.)

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