33
34
is high population density than an industrial area. For NPAHs, high risk was identified especially in non-ferrous metal industrial complexes suggesting that NPAHs having toxic coefficients were emitted in non-ferrous metal industrial complexes.
In this study, the seasonal and spatial variation were confirmed to identify the level of target compounds (PAHs, OPAHs, and NPAHs) and their potential emission sources using PAS-PUF in Ulsan, which is large industrial area. These results can be used as basic data for domestic NOPAHs research in the future. However, long-term monitoring is required to clearly identify the emission source of contamination. Since PAS-PUF mainly collects gas phases, there are limitations in using diagnostic ratio and identification of long-range transport. To solve these limitations, it is necessary to predict the particulate concentration with gas-particle partitioning and correct the concentration.
Further studies on particulate NOPAH using an active air sampler are also necessary to clearly identify gas-particle distribution on NOPAHs in Korea.
35
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Supplementary information
Figure S1. Chromatograms of calibration standard and real sample.
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Table S1. List of physicochemical properties of target compounds consisting of chemical names, abbreviations, CAS number, MW: molecular weight, H:
Henry’s law constant, boiling point, melting point, KOA: octanol-air partition coefficient, U: Internal energy. (EPI SuiteTM 4.1 (US EPA), Vuong et al.
(2022))
No. Compound Abbreviation CAS number MW
(g/mol)
log H (Pa·m3/mol)
Boiling point (°C)
Melting point
(°C) Log KOA dUOA (J/mol) Parent PAHs
1 Fluorene Flu 86-73-7 166 0.23 292.6 63.7 7.456 65.55
2 Phenanthrene Phe 1985-01-08 178 0.716 327.3 78.1 7.648 56.5
3 Anthracene Ant 120-12-7 178 0.716 327.3 78.1 7.694 57.04
4 Fluoranthene Flt 206-44-0 202 –0.075 371.9 119.9 8.711 68.43
5 Pyrene Pyr 129-00-0 202 –0.075 371.9 119.9 9.112 78.79
6 Benzo[c]phenanthrene BcP 195-19-7 228 –0.294 399.2 136 10.19 85.04
7 Benz[a]anthracene BaA 56-55-3 228 –0.294 399.2 136 10.31 86.01
8 Chrysene Chr 218-01-9 228 –0.294 399.2 136 10.34 86.24
9 Benzo[b]fluoranthene BbF 205-99-2 252 –1.086 442.8 169.4 11.44 97.55
10 Benzo[j]fluoranthene BjF 205-82-3 252 –1.086 442.8 169.4 11.44 97.55
11 Benzo[k]fluoranthene BkF 207-08-9 252 –1.086 442.8 169.4 11.49 98.12
12 7,12-Dimethylbenz[a]anthracene 7,12-DMBaA 57-97-6 256 –0.208 422.4 153.9 11.44 97.55
13 Benz[e]pyrene BeP 192-97-2 252 –1.086 442.8 169.4 11.66 99.6
14 Benz[a]pyrene BaP 50-32-8 252 –1.086 442.8 169.4 11.7 99.94
15 3-Methylcholanthrene 3-MCA 56-49-5 268 –0.521 438.3 167 12.14 104.7
16 Indeno[1,2,3-c,d]pyrene IcdP 193-39-5 276 –1.876 486.3 200 12.59 108.3
17 Dibenz[a,h]anthracene DBahA 53-70-3 278 –1.305 470.1 180.5 12.74 110
18 Benzo[g,h,i]perylene BghiP 191-24-2 276 –1.876 486.3 200 12.73 109.5
19 Dibenzo[a,i]pyrene DBaiP 189-55-9 302 –2.096 513.7 215.7 13.712 115.55
20 Dibenzo[a,h]pyrene DBahP 189-64-0 302 –2.096 513.7 215.7 13.712 115.55
21 Dibenzo[a,l]pyrene DBalP 191-30-0 302 –2.096 513.7 215.7 13.712 115.55
44 NPAHs
1 1-Nitronaphthalene 1-NNap 86-57-7 173 -0.678 309.6 92.9 7.716 79.37
2 2-Nitronaphthalene 2-NNap 581-89-5 173 -0.678 309.6 92.9 7.913 81.8
3 5-Nitroacenaphthene 5-Nace 602-87-9 211 -1.175 355.2 126.9 8.702 78.86
4 2-Nitrofluorene 2-NFlu 607-57-8 223 -1.688 384 141.6 9.1796 81.36
5 9-Nitroanthracene 9-NAnt 602-60-8 223 -1.688 384 141.6 9.06 72.81
6 3-Nitrophenanthrene 3-NPhe 17024-19-0 223 -1.688 384 141.6 9.216 74.6
7 9-Nitrophenanthrene 9-NPhe 954-46-1 223 -1.688 384 141.6 9.456 77.01
8 2-Nitrofluoranthene 2-NFlt 13177-29-2 247 -2.699 427.5 170.6 9.693 79.66
9 3-Nitrofluoranthene 3-NFlt 892-21-7 247 -2.699 427.5 170.6 10.72 89.99
10 1-Nitropyrene 1-NPyr 5522-43-0 247 -2.699 427.5 170.6 10.73 89.99
11 2-Nitropyrene 2-NPyr 57835-92-4 247 -2.699 454.9 186.6 10.6124 88.87
12 4-Nitropyrene 4-NPyr 789-07-1 247 -2.699 454.9 186.6 10.87 91.33
13 7-Nitrobenz(a)anthracene 7-NBaA 20268-51-3 273 -7.703 454.9 186.6 11.53 97.91
14 6-Nitrochyrsene 6-NChr 7496-02-08 273 -7.703 454.9 186.6 11.82 100.7
15 1,3-Dinitropyrene 1,3-DNP 75321-20-9 292 -9.889 483.2 204.7 12.4034 98.26
16 1,6-Dinitropyrene 1,6-DNP 42397-64-8 292 -9.889 483.2 204.7 12.4034 98.26
17 1,8-Dinitropyrene 1,8-DNP 42397-65-9 292 -9.889 483.2 204.7 12.4034 98.26
OPAHs
1 1,4-Naphthalenedione NAD 130-15-4 158 –3.701 301.2 82.9 6.784 66.94
2 1-Napthaldehyde NAQ 66-77-3 156 –0.876 291.1 55.3 7.245 73.14
3 9-Fluorenone FLO 486-25-9 180 –1.164 331.7 99.5 8.254 85.54
4 9-Xanthone XAT 90-47-1 196 –1.710 333.5 101.2 8.745 91.14
5 9,10-Anthracenedione ANQ 84-65-1 208 –3.492 363.6 127.6 8.519 66.81
6 2-Methyl-9,10-Anthracenedione MANQ 1984-11-07 208 –3.564 377.7 133.8 9.091 73.26
7 11-Benzo[a]fluorenone BaFL 479-79-8 230 –2.174 403.2 148.5 9.878 80.91
8 7-Benz[d,e]anthracenone BENZ 1982-05-03 230 –2.174 403.2 148.5 10.3 84.79
9 7,12-Benz[a]anthracenedione BaAD 2498-66-0 258 –4.503 434.5 173 10.63 88.08
45
Table S2. Comparison of total mean concentration of PAHs (ng/m3), OPAHs (ng/m3), and NPAHs (pg/m3) in other studies.
Location Types of sampling sites Sampling period Sampling method
PAHs (ng/m3)
OPAHs (ng/m3)
NPAHs
(pg/m3) Reference Ulsan, Korea Industrial, Urban, Rural 2016.03 - 2017.03 Passive 14.14±6.97 3.21±2.15 159.88±68.22 This study Shanxi and Shandong, China Town, Countryside,
Megacity 2011.06 - 2011.08 Passive 294 50-3740 (Lin et al.,
2015)
Alberta, Canada Oil sand area 2014.04 - 2014.05 Passive 0.05-1.32 20.9-47.8 (Jariyasopit et
al., 2016) Pokhara, Birgunj,
Kathmandu, and Biratnagar of Nepal
Urban, Industrial,
residential 2014 Passive 7.03 0.44-106 1.96-276 ng/m3 (Yadav et al.,
2018)
Alberta, Canada Oil sand area 2013.10-2016.02 Passive 400-2400
pg/m3 20-250 (Vasiljevic et al., 2021) Toronto, Canada
Background, Residential, Traffic, Urban, and
Industrial
2016.08-2017.08 Passive 5.0-27.7 0.573-3.92 22.3-147 (Jariyasopit et al., 2019)
Alberta, Canada Oil sand area 2015.10-2015.11 Passive 0.21-1.48 8.42-170 (Jariyasopit et
al., 2018) Marseille, France Urban, Sub-urban, and
Rural 2004,07 Active
(PM10+PUF) 4.4-21.4 1.3-6.3 30-710 (Albinet et al., 2007)
Paris, France Traffic, Suburban 2009 Active 0.53-7.05 113.2-1503.8
pg/m3 25.4-175.4
(Ringuet, Albinet, et al.,
2012) Beijing, China Megacity 2008.07-2008.08 Active 10.5-22.1 0.69-.1.03 421.3-792.1 (Wang et al.,
2011)
Seoul, Korea Megacity 2020.05-2020.06 Active 3.96 ± 3.36 5.49 ± 2.40 (Shin et al.,
2022)
Birmingham, UK Traffic roadside 2010.02 Active
(PM10+PUF) 87.6 50.4
(Delgado- Saborit et al.,
2013)
Alpine valleys Suburban 2002-2003 Active
(PM10+PUF) 4.6-17.3 120-520 (Albinet et al.,
2008)
Tianjin, China Traffic roadside 2016.11 Active
(PM2.5) 6.86-15.84 3.98-18.44 482-3766 (Wang et al., 2022)
46
Table S3. Result of correlation analysis between NOPAHs and CAPs at spring.
Table S4. Result of correlation analysis between NOPAHs and CAPs at summer.
47
Table S5. Result of correlation analysis between NOPAHs and CAPs at Fall.
Table S6. Result of correlation analysis between NOPAHs and CAPs at Winter.
48
Figure S2. Spatial distribution of NO2 in Ulsan, in (a) spring, (b) summer, (c) fall, and (d) winter.
Figure S3. Spatial distribution of population density (people/km2) in Ulsan.
49
Table S7. Result of correlation analysis between PAHs and OPAHs.
Table S8. Result of correlation analysis between PAHs and NPAHs.
Table S9. Result of correlation analysis between NPAHs and OPAHs.
50
Acknowledgement
졸업이 다가오니 2013년 UNIST에 입학한 후 저의 20대의 기억들이 새록새록 생각납니다. 고등학생 때 생명공학에 관심이 있어 입학하였지만, 대학생 생활을 하면서 환경에 관심이 생겨 학과를 변경하여 도시환경공학부에 들어오게 되었습니다. 여러 일이 있어 군대를 다녀온 후, 저의 대학생 지도교수님인 최성득 교수님 연구실(환경분석화학 연구실, EACL)에 인턴으로 들어왔습니다. 인턴 생활 동안 환경시료채취와 데이터 수집 및 해석을 해가며 환경연구에 더욱 흥미가 생겨 대학원을 진학하였습니다. 최성득 교수님께서는 부족한 저를 받아주시고 연구할 수 있는 환경을 제공해주셨고 삶에 대해서도 아낌없는 조언을 해주셨습니다. 저를 한 단계 더 나아가게 해주신 최성득 교수님께 깊은 감사를 전하고 싶습니다.
석사졸업논문과 논문발표에 심사위원을 참여해주신 장윤석 교수님과 송창근 교수님에게 감사를 표합니다. 바쁘신 시간을 내어 주셔서 제가 생각하지 못한 조언과 논평을 해주셔서 정말 감사합니다.
교수님들 덕분에 학위논문을 더 의미 있게 보강하여 마무리 지을 수 있었습니다.
EACL에 들어온 지 어느덧 2년 6개월이 지나며, 많은 사람을 만났습니다. 같이 석사과정을 들어와 힘든 시간 이겨낸 종현, 민재부터 연구실 선후배로 만난 민규 형, 성준 형, 상진 형, 혜경 누나, 호영, 인규, 나라, 혜지, 손지민 선생님, 상화, 민지, 정태, Quang, Tien, Renato, Bala, Nirmala, Onynine, Phu까지 같이 연구하고 토론할 수 있어서 정말 즐겁고 덕분에 의미 있는 시간을 보낼 수 있었습니다.
선배님들에게 환경연구를 하기 위한 시료채취부터 데이터 해석, 연구실 생활까지 많은 것을 보고 배울 수 있었습니다. 후배 친구들은 같이 실험하고 제 졸업 실험까지 도와줘서 힘든 시기를 이겨낼 수 있게 해줘서 모두 정말 고맙고 감사합니다.
고등학생 시절부터 언제나 응원해준 주원, 민호, 현수, 주용이부터 대학생 시절부터 꾸준히 만나며 서로에게 거침없는 조언들을 해준 호영, 창근, 성호도 정말 고맙고 군대 시절 맞후임으로 인연이 생겨 나와서도 계속 연락해주고 존중해준 상기까지, 다들 저에게 큰 힘이 되어 주셔서 정말 감사합니다.
마지막으로, 사랑하는 연휘에게 바쁜 대학원생 생활을 이해해주고 응원해주고 사랑해줘서 정말 고마웠습니다. 연인으로서 군대, 대학원을 기다려줘서 언제나 큰 힘이 되어줬습니다. 앞으로 남은 인생은 제가 옆에서 큰 버팀목으로 사랑해드리겠습니다.
이 논문을 시작으로 저는 앞으로 더 나은 삶을 살아가기 위해 노력하겠습니다. 많은 분에게 배운 지식과 지혜를 바탕으로 한 치 앞도 알 수 없는 미래를 개척해 나아가겠습니다. 그동안 정말 감사했습니다.
긴 글 읽어 주셔서 감사합니다.