DOI QR코드

DOI QR Code

한반도 서부유입권역에서 대기 중 에어로졸 성분의 화학적 특성 연구 II. 입자의 산성도 및 산화 특성

A Study on Chemical Characteristics of Aerosol Composition at West Inflow Regions in the Korean Peninsula II. Characteristics of Inorganic Aerosol Acidity and Organic Aerosol Oxidation

  • 최진수 (국립환경과학원 기후대기연구부 대기환경연구과) ;
  • 김정호 (에이피엠 엔지니어링(주)) ;
  • 이태형 (한국외국어대학교 환경학과) ;
  • 최용주 (한국외국어대학교 환경학과) ;
  • 박태현 (한국외국어대학교 환경학과) ;
  • 안준영 (국립환경과학원 기후대기연구부 대기환경연구과) ;
  • 박진수 (국립환경과학원 기후대기연구부 대기환경연구과) ;
  • 김현재 (국립환경과학원 기후대기연구부 대기환경연구과) ;
  • 구윤서 (안양대학교 환경에너지공학과) ;
  • 김신도 (서울시립대학교 환경공학과) ;
  • 홍유덕 (국립환경과학원 기후대기연구부 대기환경연구과) ;
  • 홍지형 (국립환경과학원 기후대기연구부 대기환경연구과)
  • Choi, Jin-Soo (Department of Air Quality Research, Climate and Air Quality Research Division, National Institute of Environmental Research) ;
  • Kim, Jeong-Ho (APM Engineering Co., Ltd.) ;
  • Lee, Tae-Hyoung (Department of Environmental Science, Hankuk University of Foreign Studies) ;
  • Choi, Yong-Joo (Department of Environmental Science, Hankuk University of Foreign Studies) ;
  • Park, Tae-Hyun (Department of Environmental Science, Hankuk University of Foreign Studies) ;
  • Ahn, Joon-Young (Department of Air Quality Research, Climate and Air Quality Research Division, National Institute of Environmental Research) ;
  • Park, Jin-Soo (Department of Air Quality Research, Climate and Air Quality Research Division, National Institute of Environmental Research) ;
  • Kim, Hyun-Jae (Department of Air Quality Research, Climate and Air Quality Research Division, National Institute of Environmental Research) ;
  • Koo, Youn-Seo (Department of Environmental and Energy Engineering, Anyang University) ;
  • Kim, Shin-Do (Department of Environmental Engineering, University of Seoul) ;
  • Hong, You-Deog (Department of Air Quality Research, Climate and Air Quality Research Division, National Institute of Environmental Research) ;
  • Hong, Ji-Hyung (Department of Air Quality Research, Climate and Air Quality Research Division, National Institute of Environmental Research)
  • 투고 : 2016.06.20
  • 심사 : 2016.09.21
  • 발행 : 2016.10.31

초록

We examined acidity state of inorganic aerosol and oxidation state of organic aerosol by High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) at Baengnyeong Super site from Jan 2012 to Dec 2013. Additionally, we carried out the analysis for the aerosol component group of organic matter ($C_xH_y$, $C_xH_yO_1$, $C_xH_yO_z$, $C_xH_yO_zN_p$) and elemental composition to calculate H/C, O/C, N/C, OM/OC and identify the oxidation state. The aerosol chemical composition in this study is dominated by sulfate ($SO_4{^{2-}}$), nitrate ($NO_3{^-}$) plays a smaller role in aerosol acidity. Ammonium ($NH_4{^+}$) was found in a formation of $(NH_4)_3H(SO_4)_2$. However, the binding formations of $NH_4NO_3$ and $NH_4Cl$ increase in the winter. $C_xH_yO_1$ indicating the oxidized state of $PM_{1.0}$ has the highest ratio of 41% while $C_xH_y$ indicating the non-oxidized state has a lower ratio of 36%, meaning that the oxidation level of $PM_{1.0}$ in Baengnyeong Island is high. The ratio between H/C and O/C was 1.33 and 0.78 respectively, showing the characteristic of LV-OOA (Low volatility-Oxygenated Organic Aerosol). Acidic and oxidized aerosols sampled during this field study were largely anthropogenic in origin from Chinese continent and photochemically aged.

키워드

참고문헌

  1. Aiken, A.C., P.F. Decarlo, J.H. Kroll, D.R. Worsnop, J.A. Huffman, K.S. Docherty, I.M. Ulbrich, C. Mohr, J.R. Kimmel, D. Sueper, Y.L. Sun, Q. Zhang, A. Trimborn, M. Northway, P.J. Ziemann, M.R. Canagaratna, T.B. Onasch, M.R. Alfarra, A.S.H. Prevot, J. Dommen, J. Duplissy, A. Metzger, U. Baltensperger, and J.L. Jimenez (2008) O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high resolution time-of-flight aerosol mass spectrometry, Environmental Science and Technology, 42(12), 4478-4485. https://doi.org/10.1021/es703009q
  2. Alfarra, M.R., H. Coe, J.D. Allan, K.N. Bower, H. Boudries, M.R. Canagaratna, J.L. Jimenez, J.T. Jayne, A. Garforth, S.M. Li, and D.R. Worsnop (2004) Characterization of Urban and Regional Organic Aerosols In the Lower Fraser Valley Using Two Aerosol Mass Spectrometers, Atmospheric Environment, 38(34), 5745-5758. https://doi.org/10.1016/j.atmosenv.2004.01.054
  3. Baker, K.R. and K.M. Foley (2011) A nonlinear regression model estimating single source concentrations of primary and secondarily formed $PM_{2.5}$, Atmospheric Environment, 45(22), 3758-3767. https://doi.org/10.1016/j.atmosenv.2011.03.074
  4. Bian, Q., X.H.H. Huang, and J.Z. Yu (2014) One-year observations of size distribution characteristics of major aerosol constituents at a coastal receptor site in Hong Kong - Part1: Inorganic ions and oxalate, Atmospheric Chemistry and Physics, 14(17), 9013-9027. https://doi.org/10.5194/acp-14-9013-2014
  5. Boudries, H., M.R. Canagaratna, J.T. Jayne, M.R. Alfarra, J. Allan, K.N. Bower, H. Coe, S.C. Pryor, J.L. Jimenez, J.R. Brook, S. Li, and D.R. Worsnop (2004) Chemical and physical processes controlling the distribution of aerosol in the Lower Fraser Valley, Canada, during the Pacific 2001 field campaign, Atmospheric Environment, 38(34), 5759-5774. https://doi.org/10.1016/j.atmosenv.2004.01.057
  6. Choi, J.S., J.H. Kim, J.Y. Ahn, J.S. Park, Y.S. Koo, G.H. Yoon, and S.D. Kim (2013) A case study on the high mass loading aerosol observed using an aerodyne ToFAMS in Baegryung Island, May 2011, Journal of Korean Society of Urban Environment, 13(1), 19-32. (in Korean with English abstract)
  7. Fisher, J., D.J. Jacob, Q. Wang, R. Bahreini, C.C. Carouge, M.J. Cubison, J.E. Dibb, T. Diehl, J.L. Jimenez, E.M. Leibensperger, M.B.J. Meinders, H.O.T. Pye, P.K. Quinn, S. Sharma, A. van Donkelaar, and R.M. Yantosca (2011) Sources, distribution, and acidity of sulfate-ammonium aerosol in the Arctic in winterspring, Atmospheric Environment, 45(39), 7301-7318. https://doi.org/10.1016/j.atmosenv.2011.08.030
  8. Heald, C.L., J.H. Kroll, J.L. Jimenez, K.S. Docherty, P.F. DeCarlo, A.C. Aiken, Q. Chen, S.T. Martin, D.K. Farmer, and P. Artaxo (2010) A simplified description of the evolution of organic aerosol composition in the atmosphere, Geophysical Research Letters, 37(8), L08803, doi:10.1029/2010GL042737.
  9. Jeon, H.E., J.S. Park, H.J. Kim, M.Y. Sung, J.S. Choi, Y.D. Hong, and J.H. Hong (2015) The characteristics of $PM_{2.5}$ concentration and chemical composition of Seoul metropolitan and inflow background area in Korea peninsula, Journal of Korean Society of Urban Environment, 15(3), 261-271. (in Korean with English abstract)
  10. Jimenez, J.L., M.R. Canagaratna, N.M. Donahue, A.S.H. Prevot, Q. Zhang, J.H. Kroll, P.F. DeCarlo, J.D. Allan, H. Coe, N.L. Ng, A.C. Aiken, K.S. Docherty, I.M. Ulbrich, A.P. Grieshop, A.L. Robinson, J. Duplissy, J.D. Smith, K.R. Wilson, V.A. Lanz, C. Hueglin, Y.L. Sun, J. Tian, A. Laaksonen, T. Raatikainen, J. Rautiainen, P. Vaattovaara, M. Ehn, M. Kulmala, J.M. Tomlinson, D.R. Collins, M.J. Cubison, E.J. Dunlea, J.A. Huffman, T.B. Onasch, M.R. Alfarra, P.I. Williams, K. Bower, Y. Kondo, J. Schneider, F. Drewnick, S. Borrmann, S. Weimer, K. Demerjian, D. Salcedo, L. Cottrell, R. Griffin, A. Takami, T. Miyoshi, S. Hatakeyama, A. Shimono, J.Y. Sun, Y.M. Zhang, K. Dzepina, J.R. Kimmel, D. Sueper, J.T. Jayne, S.C. Herndon, A.M. Trimborn, L.R. Williams, E.C. Wood, A.M. Middlebrook, C.E. Kolb, U. Baltensperger, and D.R. Worsnop (2009) Evolution of organic aerosols in the atmosphere, Science, 326(5959), 1525-1529. https://doi.org/10.1126/science.1180353
  11. Kim, J.H., J.S. Choi, J. Oh, J.Y. Ahn, J.S. Park, G.H. Yoon, S.D. Kim, and J.S. Han (2014) Characteristics of Organic Components on the High Mass Loading Aerosol observed at Baengnyeong Island, May 2011, Journal of Korean Society of Urban Environment, 14(3), 203-211. (in Korean with English abstract)
  12. Kim, J.H., J.S. Choi, J.Y. Ahn, J.S. Han, G.H. Yoon, and S.D. Kim (2013) A Study on the Mass Spectrums of the Main and Side-stream Smoke Aerosol of Cigarette using an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer, Journal of Korean Society of Urban Environment, 13(3), 243-252. (in Korean with English abstract)
  13. Kim, J.H., T.H. Lee, G.H. Yoon, J.J. Lee, B.R. Seo, J.S. Park, J.Y. Ahn, and S.D. Kim (2012) Study of cigarette smoke aerosol particles in indoor environment using an High Resolution Time of Flight Aerosol Mass Spectometry (HR-ToF-AMS), Journal of Korean Society of Urban Environment, 12(2), 99-106. (in Korean with English abstract)
  14. Langner, J. and H. Rodhe (1991) A global scale three-dimensional model of the tropospheric sulfur cycle, Journal of Atmospheric Chemistry, 13(3), 225-263. https://doi.org/10.1007/BF00058134
  15. Lee, T.H., J.S. Choi, G.W. Lee, J.Y. Ahn, J.S. Park, A.A. Samuel, S.M. Misha, Y.J. Choi, and Y.M. Chung (2015) Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer, Atmospheric Environment, 120, 297-306. https://doi.org/10.1016/j.atmosenv.2015.08.038
  16. Long, S., J. Zeng, Y. Li, L. Bao, L. Cao, K. Liu, L. Xu, J. Lin, W. Liu, G. Wang, J. Yao, C. Ma, and Y. Zhao (2014) Characteristics of secondary inorganic aerosol and sulfate species in size fractionated aerosol particles in Shanghai, Journal of Environmental Science, 26(5), 1040-1051. https://doi.org/10.1016/S1001-0742(13)60521-5
  17. Middlebrook, A.M., D.M. Murphy, and D.S. Thomson (1998) Observations of organic material in individual marine particles at Cape Grim during the first aerosol characterization experiment (ACE 1), Journal of Geophysical Research Atmospheres, 103(D13). 16475-16483, doi: 10.1029/97JD03719.
  18. Ng, N.L., M.R. Canagaratna, J.L. Jimenez, P.S. Chhabra, J.H. Seinfeld, and D.R. Worsnop (2011) Changes in organic aerosol composition with aging inferred from aerosol mass spectra, Atmospheric Chemistry and Physics, 11(13), 6465-6474. https://doi.org/10.5194/acp-11-6465-2011
  19. Ng, N.L., M.R. Canagaratna, Q. Zhang, J.L. Jimenez, J. Tian, I.M. Ulbrich, J.H. Kroll, K.S. Docherty, P.S. Chhabra, R. Bahreini, S.M. Murphy, J.H. Seinfeld, L. Hildebrandt, N.M. Donahue, P.F. DeCarlo, V.A. Lanz, A.S.H. Prevot, E. Dinar, Y. Rudich, and D.R. Worsnop (2010) Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry, Atmospheric Chemistry and Physics, 10(10), 4625-4641. https://doi.org/10.5194/acp-10-4625-2010
  20. Park, J.S., I.H. Song, S.M. Park, H.J. Shin, and Y.D. Hong (2015) Characteristics of Submicron Particle during High Concentration Episodes in Spring, 2014 at Seoul, Korea, using the Aerosol Mass Spectrometer, Journal of Korean Society for Environmental Analysis, 18(1), 12-25. (in Korean with English abstract)
  21. Salcedo, D., A. Laskin, V. Shutthanandan, and J.L. Jimenez (2012) Feasibility of the Detection of Trace Elements in Particulate Matter using Online High Resolution Aerosol Mass Spectrometry, Aerosol Science and Technology, 46, 1187-1200. https://doi.org/10.1080/02786826.2012.701354
  22. Salcedo, D., T.B. Onasch, M.R. Canagaratna, Q. Zhang, J.A. Huffman, P.F. DeCarlo, J.T. Jayne, P. Mortimer, D.R. Worsnop, C.E. Kolb, K.S. Johnson, B. Zuberi, L.C. Marr, R. Volkamer, L.T. Molina, B. Cardenas, R.M. Bernabe, C. Marquea, J.S. Gaffney, N.A. Marley, A. Laskin, V. Shutthanandan, Y. Xie, W. Brune, R. Lesher, T. Shirley, and J.L. Jimenex (2006) Characterization of ambient aerosols in Mexico City during the MCMA-2003 campaign with Aerosol Mass Spectrometry: results from the CENICA Supersite, Atmospheric Chemistry and Physics, 6(4), 925-946. https://doi.org/10.5194/acp-6-925-2006
  23. Setyan, A., Q. Zhang, M. Merkel, W.B. Knighton, Y. Sun, C. Song, J.E. Shilling, T.B. Onasch, S.C. Herndon, D.R. Worsnop, J.D. Fast, R.A. Zaveri, L.K. Berg, A. Wiedensohler, B.A. Flowers, M.K. Dubey, and R. Subramanian (2012) Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES, Atmospheric Chemistry and Physics, 12(17), 8131-8156. https://doi.org/10.5194/acp-12-8131-2012
  24. Shaw, R.W. and H. Rodhe (1982) Non-photochemical oxidation of $SO_2$ in regionally polluted air during winter, Atmospheric Environment, 16(12), 2879-2888. https://doi.org/10.1016/0004-6981(82)90038-5
  25. Shen, X.H., T.Y. Lee, J. Guo, X.F. Wang, P.H. Li, P.J. Xu, Y. Wang, Y. Ren, W. Wang, T. Wang, S.A. Cam, and J.L. Collet (2012) Aqueous phase sulfate production in clouds in eastern China, Atmospheric Environment, 62, 502-511. https://doi.org/10.1016/j.atmosenv.2012.07.079
  26. Sievering, H., J. Boatman, J. Galloway, W. Keene, Y. Kim, M. Luria, and J. Ray (1991) Heterogenous sulfer conversion in sea-salt aerosol particles: the role of aerosol water content and size distribution, Atmospheric Environment, 25(8), 1479-1487. https://doi.org/10.1016/0960-1686(91)90007-T
  27. Song, C.H. and G.R. Carmichael (1999) The aging process of naturally emitted aerosol (sea-salt and mineral aerosol) during long range transport, Atmospheric Environment, 33(14), 2203-2218. https://doi.org/10.1016/S1352-2310(98)00301-X
  28. Sueper, D. (2009) ToF-AMS high resolution analysis software, Online available at: http://cires.colorado.edu/jimenez-group/ToFAMSResources/ToFSoftware/indez.html.
  29. Sun, J.Y., Q. Zhang, M.R. Canagaratna, Y.M. Zhang, N.L. Ng, Y.L. Sun, J.T. Jayne, X.C. Zhang, X.Y. Zhang, and D.R. Worsnop (2010) Highly time- and size resolved characterization of submicron aerosol particle in Beijing using an Aerodyne Aerosol Mass Spectrometer, Atmospheric Environment, 44(1), 131-140. https://doi.org/10.1016/j.atmosenv.2009.03.020
  30. Sun, Y.L., G.S. Zhuang, A. Tang, Y. Wang, and Z.S. An (2006) Chemical Characteristics of PM2.5 and PM10 in Haze-Fog Episodes in Beijing, Environmental Science and Technology, 40(10), 3148-3155. https://doi.org/10.1021/es051533g
  31. Sun, Y.L., Q. Zhang, J.J. Schwab, K.L. Demerjian, W.N. Chen, M.S. Bae, H.M. Hung, O. Hogrefe, B. Frank, O.V. Rattigan, and Y.C. Lin (2011) Characterization of the sources and processes of organic and inorganic aerosols in new york city with a high-resolution time-of-flight aerosol mass spectrometer, Atmospheric Chemistry and Physics, 11(4), 1581-1602. https://doi.org/10.5194/acp-11-1581-2011
  32. Takegawa, N., T. Miyakawa, K. Kawamura, and Y. Kondo (2007) Contribution of Selected Dicarboxylic and ${\omega}$-Oxocarboxylic Acids in Ambient Aerosol to the m/z 44 Signal of an Aerodyne Aerosol Mass Spectrometer, Aerosol Science and Technology, 41(4), 418-437. https://doi.org/10.1080/02786820701203215
  33. Takegawa, N., T. Miyakawa, Y. Kondo, J.L. Jimenez, Q. Zhang, D.R. Worsnop, and M. Fukuda (2006) Seasonal and diurnal variations of submicron organic aerosol in Tokyo observed using the Aerodyne aerosol mass spectrometer, Journal of Geophysical Research Atmospheres, 111(D11), D11206, doi:10.1029/2005JD006515.
  34. Topping, D., H. Coe, G. McFiggans, R. Burgess, J. Allan, M.R. Alfarra, K. Bower, T.W. Choularton, S. Decesari, and M.C. Facchini (2004) Aerosol chemical characteristics from sampling conducted on the Island of Jeju, Korea during ACE Asia, Atmospheric Environment, 38(14), 2111-2123. https://doi.org/10.1016/j.atmosenv.2004.01.022
  35. Xu, J., Q. Zhang, M. Chen, X. Ge, J. Ren, and D. Qin (2014) Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry, Atmospheric Chemistry and Physics, 14(23), 12593-12611. https://doi.org/10.5194/acp-14-12593-2014
  36. Zhang, J.K., Y. Sun, Z.R. Liu, D.S. Ji, B. Hu, Q. Liu, and Y.S. Wang (2014) Characterization of submicron aerosols during a month of serious pollution in Beijing, 2013, Atmospheric Chemistry and Physics, 14(6), 2887-2903. https://doi.org/10.5194/acp-14-2887-2014
  37. Zhang, Q., D.R. Worsnop, M.R. Canagaratna, and J.L. Jimenez (2005a) Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols, Atmospheric Chemistry and Physics, 5(12), 3289-3311. https://doi.org/10.5194/acp-5-3289-2005
  38. Zhang, Q., J.L. Jimenez, D.R. Worsnop, and M.R. Canagaratna (2007) A Case Study of Urban Particle Acidity and its Effect on Secondary Organic Aerosol, Environmental Science and Technology, 41(9), 3213-3219. https://doi.org/10.1021/es061812j
  39. Zhang, Q., M.R. Canagaratna, J.T. Jayne, D.R. Worsnop, and J.L. Jimenez (2005b) Time and size resolved chemical composition of submicron particles in Pittsburgh: Implications for aerosol sources and processes, Journal of Geophysical Research Atmospheres, 110(D7), D07S09, doi:10.1029/2004JD004649.

피인용 문헌

  1. Spacial Distribution of PM1.0 Major Compounds from Long Range Transport at the Baegryungdo Super Site: Relationship between PSCF and Cluster Analysis vol.33, pp.4, 2017, https://doi.org/10.5572/KOSAE.2017.33.4.411