Asian Journal of Atmospheric Environment

Korean Society for Atmospheric Environment (한국대기환경학회)
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Development of HPLC Determination Method for Trace Levels of 1-, 2-Nitropyrenes and 2-Nitrofluoranthene in Airborne Particulates and Its Application to Samples Collected at Noto Peninsula

  • Hayakawa, Kazuichi (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Tang, Ning (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Sato, Kosuke (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Izaki, Akihiko (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Tatematsu, Michiya (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Hama, Hirotaka (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Li, Ying (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Kameda, Takayuki (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University) ;
  • Toriba, Akira (Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University)
  • Received : 2010.11.18
  • Accepted : 2011.03.10
  • Published : 2011.09.30
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Abstract

1-Nitropyrene (1-NP), 2-NP and 2-nitrofluoranthene (2-NFR) are useful markers for studying the atmospheric behaviors of polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs). However, present methods for measuring trace levels of these compounds are lesssensitive and laborious. Here we describe several improvements to a previously reported high-performance liquid chromatography-chemiluminescence detection system that allows it to determine trace levels of 1-, 2-NPs and 2-NFR. The proposed system was equipped with a reducer column packed with Pt/Rh instead of zinc whose life-time was limited. The combination of Cosmosil MS-II (monomeric ODS) and AR-II (polymeric ODS) columns was used instead of polymeric ODS columns as the separator column to improve the separation. An ethanol mixture with acetate buffer (pH 5.5) was used in place of an acetonitrile mixture with the same buffer to activate the reducer column. The same ethanol mixture was used as the mobile phase for the clean-up column. The switching time of the column switching valve was optimized to concentrate the amino-derivatives of above NPAHs quantitatively on the concentrator column. The concentrations of bis(2,4,6-trichlorophenly) oxalate and hydrogen peroxide in the chemiluminescence reagent solution were optimized to 0.4 mM and 30 mM, respectively, to increase the sensitivity. Under the above conditions, the detection limits (S/N=3) of 1-, 2-NPs and 2-NFR were 1 fmol (0.25 pg), 10 fmol (2.5 pg) and 4 fmol (1 pg), respectively. The proposed system was effectively used to determine trace levels of 1-, 2-NPs and 2-NFR in airborne particulates collected at Noto Peninsula. The atmospheric concentrations of 1-, 2-NPs and 2-NFR were not more than sub pg $m^{-3}$ levels. They were higher in winter (January) than in summer (July). In both seasons, the concentrations were in decreasing order, [2-NFR]>[1-NP]>[2-NP].

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References

  1. Arey, J., Zielinska, B., Atkinson, R., Winer, A.M., Ramdahl, T., Pitts, J.N. Jr. (1986) The formation of nito-PAH from the gas-phase reactions of fluoranthene and pyrene with OH radical in the presence of NOx. Atmospheric Environment 20, 2339-2345. https://doi.org/10.1016/0004-6981(86)90064-8
  2. Hattori, T., Tang, N., Tamura, K., Hokoda, A., Yang, X.-Y., Igarashi, K., Ohno, M., Okada, Y., Toriba, A., Hayakawa, K. (2007) Profiles of particulate-bound polycyclic aromatic hydrocarbons and their nitrated derivatives in three typical cities, Liaoning Province, China. Environmental Forensics 8(1 & 2), 165-172. https://doi.org/10.1080/15275920601180701
  3. Hayakawa, K., Kitamura, R., Butoh, M., Imaizumi, N., Miyazaki, M. (1991) Determination of Diamino- and Aminopyrenes by High-Performance Liquid Chromatography with Chemiluminescence Detection. Analytical Sciences 7, 573-577. https://doi.org/10.2116/analsci.7.573
  4. Hayakawa, K., Terai, N., Suzuki, K., Dinning, P.G., Yamada, M., Miyazaki, M. (1993) Chromatographic Determination Method for 1-Nitropyrene and Its Metabolites in Biological Samples with Fluorescence Detection after On-line Reduction. Biomedical Chromatography 7, 262-266. https://doi.org/10.1002/bmc.1130070505
  5. Hayakawa, K., Murahashi, T., Butoh, M., Miyazaki, M. (1995) Determination of 1,3-, 1,6-, and 1,8-Dinitropyrenes and 1-Nitropyrene in Urban Air by High-Performance Liquid Chromatography Using Chemiluminescence Detection. Environmental Science & Technology 29, 928-932. https://doi.org/10.1021/es00004a012
  6. Hayakawa, K., Noji, K., Tang, N., Toriba, A., Kizu, R. (2001) A High-Performance Liquid Chromatographic System Equipped with Reducer and Concentrator Columns for Determination of Trace Levels of Nitropolycyclic Aromatic Hydrocarbons in Extracts from Diesel- Engine Exhaust Particulates. Analytica Chimica Acta 445, 205-212. https://doi.org/10.1016/S0003-2670(01)01279-X
  7. Imaizumi, N., Hayakawa, K., Suzuki, Y., Miyazaki, M. (1990) Determination of Nitrated Pyrenes and Their Derivatives by High-Performance Liquid Chromatography with Chemiluminescence Detection after Online Electrochemical Reduction. Noriko Imaizumi, Biomedical Chromatography 4, 108-112. https://doi.org/10.1002/bmc.1130040307
  8. Kizu, R., Ishii, K., Kobayashi, J., Hashimoto, T., Koh, E., Namiki, M., Hayakawa, K. (2000) Antiandrogenic Effect of Crude Extract of C-Heavy Oil. Materials Science & Engineering C 12(1-2), 97-102. https://doi.org/10.1016/S0928-4931(00)00165-X
  9. Motoyama, Y., Bekki, K., Chung, S.-W., Tang, N., Kameda, T., Toriba, A., Taguchi, K., Hayakawa, K. (2009) Oxidative stress more strongly induced by ortho- than para-quinoid polycyclic aromatic hydrocarbons in A549 cells. Journal of Health Science 55(5), 845-850. https://doi.org/10.1248/jhs.55.845
  10. Murahashi, T., Hayakawa, K. (1997) A Sensitive Method for the Determination of 6-Nitrochrysene, 2-Nitrofluoranthene and 1-, 2- and 4-Nitropyrenes in Airborne Particulates Using High-Performance Liquid Chromatography with Chemiluminescence Detection. Analytica Chimica Acta 343, 251-257. https://doi.org/10.1016/S0003-2670(96)00632-0
  11. Murahashi, T., Kizu, R., Kakimoto, H., Toriba, A., Hayakawa, K. (1999) 2-Nitrofluoranthene, 1-, 2- and 4-Nitropyrenes and 6-Nitrochrysene in Diesel-Engine Exhaust and Airborne Particulates. Journal of Health Science 45(5), 244-250. https://doi.org/10.1248/jhs.45.244
  12. Tang, N., Toriba, A., Kizu, R., Hayakawa, K. (2003) Improvement of an Automatic HPLC System for Nitropolycyclic Aromatic Hydrocarbons: Removal of an Interfering Peak and Increase in the Number of Analytes. Analytical Sciences 19(2), 249-253. https://doi.org/10.2116/analsci.19.249
  13. Tang, N., Taga, R., Hattori, T., Toriba, A., Kizu, R., Hayakawa, K. (2005) Simultaneous determination of twentyone mutagenic nitropolycyclic aromatic hydrocarbons by high-performance liquid chromatography with chemiluminescence detection, Proceedings of the 13th International Symposium, Bioluminescence and Chemiluminescence Progress and Perspective, ed. by A. Tsuji et al., World Science, London, pp. 441-444.
  14. Tokiwa, H., Kitamori, S., Takahashi, K., Ohnishi, Y. (1980) Mutagenic and chemical assay of extracts of airborne particulates. Mutation Research 77, 99-108. https://doi.org/10.1016/0165-1218(80)90126-3
  15. Yang, X.-Y., Okada, Y., Tang, N., Matsunaga, S., Tamura, K., Kameda, T., Toriba, A., Hayakawa, K. (2007) Longrange transportation of polycyclic aromatic hydrocarbons from China to Japan. Atmospheric Environment 41(22), 2710-2718. https://doi.org/10.1016/j.atmosenv.2006.11.052

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