Jpn. Soc. Atom. Env. 50(2): (2015)

Size: px

Start display at page:

Download "Jpn. Soc. Atom. Env. 50(2): (2015)"

おさむやまのかみしゃ
5 years ago
Views:

1 PAH/NPAH 1 * Variation of Polycyclic Aromatic Hydrocarbons and Nitropolycyclic Aromatic Hydrocarbons in Airborne Particulates Collected in Japanese Capital Area Genki Suzuki 1 *, Tazuko Morikawa 2, Kiriko Kashiwakura 2, Ning Tang 3, Akira Toriba 3, Kazuichi Hayakawa 3 1 School of Phamacy, Kanazawa University, College of Medical, Pharmaceutical and Health Sciences, Kakumamachi, Kanazawa, Ishikawa , Japan 2 Japan Automobile Research Institute, 2530, Karima, Tsukuba, Ibaraki , Japan 3 Institute of Medical, Pharmaceutical and Health Sciences, Kanazawa University, Kakuma-machi, Kanazawa, Ishikawa , Japan *Corresponding author: ( ) gengen@stu.kanazawa-u.ac.jp Airborne particulates were collected in Noge and Kudan, Japan, in the summer and winter from 2006 to 2013 and in Tsukuba, Japan, in the summer and winter from 2010 to The polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by HPLC with fluorescence and chemiluminescence detections, respectively. The decreasing tendencies of the total concentrations of nine PAHs were observed at Noge and Kudan in the winter from 2006 to The decreasing tendencies of the total concentrations of three NPAHs were observed in both the summer and winter in Noge from 2006 to The decreasing tendencies of the NPAH concentrations were also observed in Kudan in the winter from 2006 to 2011 and in the summer from 2007 to The concentration ratio of 1-nitropyrene to pyrene also decreased in Noge and Kudan. As the main reason for the decrease in the urban atmospheric PAH and NPAH concentrations, the Japanese regulation of exhaust gas/particulates from automobiles was considered. Key words : Polycyclic aromatic hydrocarbon, nitropolycyclic aromatic hydrocarbon, automobile 1 (polycyclic aromatic hydrocarbon; PAH) (nitropolycyclic aromatic hydrocarbon; NPAH) PAH NPAH (International Agency for Research on Cancer; IARC) benzo a pyrene (BaP) Group 1 (Carcinogenic to humans) dibenz a,h anthracene (DBA) 6-nitrochrysene (6-NC) 1-nitropyrene (1-NP) Group 2A (Probably carcinogenic to humans) (IARC, 2014) 1,3-, 1,6-, 1,8-dinitropyrenes (DNPs) 1-NP (Ames et al., 1975; Epstein et al., 1979) PAH NPAH NPAH NPAH 1,3-, 1,6-, 1,8-DNP 1-NP 6-NC 7-nitrobenz a anthracene (7-NBaA) 6-nitrobenzo a pyrene (6-NBaP) NPAH 2-nitropyrene (2-NP) 2-nitrofluoranthene (2-NFR) (Atkinson and Arey, 1994) PAH NPAH (Hayakawa et al., 1994; Murahashi et al., 1995; Tang et al., 2005) 2008 (Morikawa and Mizohata, 2013) PAH NPAH PAH NPAH

2 118 J. Jpn. Soc. Atmos. Environ. Vol. 50 No m (Japan Automobile Research Institute; JARI) AH-600F, 566 L/min T60A20, PALL Corporation; TX40H120-WW, PALL Corporation 7.0 μm μm μm μm 1.1 μm μm JARI μm 2 μm DMSO 100 μl 10 ml PAH pyrene-d 10 (Pyr-d 10 ) benzo a pyrene-d 12 (BaP-d 12 ) NPAH 2-fluoro-7-nitrofluorene (FNF) 30 ml 5 (w/v) 20 (v/v) 2 DMSO 100 μl 900 μl HLC-DISK3, 0.45 μm PAH NPAH 2. 3 PAH NPAH PAH (Tang et al., 2005; Toriba et al., 2003) HPLC- PAH 4 fluoranthene (FR) pyrene (Pyr) benz a anthracene (BaA) chrysene (Chr) 5 benzo b fluoranthene (BbF) benzo k fluoranthene (BkF) benzo a pyrene (BaP) dibenz a,h anthracene (DBA) 6 benzo ghi perylene (BghiPe) indeno 1,2,3-c,d pyrene (IDP) 10 NPAH HPLC- (Hayakawa et al., 1991; Tang et al., 2003) NPAH 3 2-nitrofluorene (2-NF) 2-, 9-nitroanthracene (NA) 9-nitrophenanthrene (9-NPh) 4 1,3-, 1,6-, 1,8-dinitropyrene (DNP) 1-, 4-nitropyrene (NP) 3-nitrobenzanthrone (3-NBA) 1-, 3-nitrofluoranthene (NFR) 7-nitrobenz a anthracene (7-NBaA) 2- nitrotriphenylene (2-NTP) 6-nitrochrysene (6-NC) 5 6-nitrobenzo a pyrene (6-NBaP) 1-, 3-nitroperylene (NPer) PAH NPAH 3 9 PAH (FR, Pyr, BaA, Chr, BbF, BkF, BaP, BghiPe, IDP) 3 NPAH (1-NP, 7-NBaA, 6-NBaP) PAH NPAH 1/2 Fig. 1 PAH Fig. 2 NPAH PAH (Fig. 3) PAH NPAH (Kakimoto et al., 2002; Tang et al., 2002, 2005)

3 Fig. 1 Variations of total PAHs concentrations in (a) Noge, (b) Kudan and (c) Tsukuba. PAH NPAH μm (2 7 μm) ( 2 μm) PAH pmol/m pmol/m pmol/m pmol/m 3 (Fig. 1) NPAH fmol/m fmol/m fmol/m fmol/m fmol/m fmol/ m fmol/m fmol/m 3 (Fig. 2) PAH NPAH PAH pmol/m pmol/m 3, pmol/m pmol/m 3, 56.5 NPAH fmol/m fmol/m 3, fmol/m fmol/m 3, Fig. 2 Variations of total NPAHs concentrations in (a) Noge, (b) Kudan and (c) Tsukuba. PAH NPAH PAH NPAH PAH PAH PAH NPAH PAH NPAH PAH NPAH PAH NPAH (Hayakawa et al., 1994; Murahashi et al., 1995; Tang et al., 2005) 1 μm PAH NPAH (Hayakawa et al., 1995;

120 J. Jpn. Soc. Atmos. Environ. Vol. 50 No. 2 2015 Fig. 4 Variations of NO 2 and CO concentrations in Tokyo and Ibaraki. Fig. 3 Compositions of PAHs in (a) Noge, (b) Kudan and (c) Tsukuba.

4 120 J. Jpn. Soc. Atmos. Environ. Vol. 50 No Fig. 4 Variations of NO 2 and CO concentrations in Tokyo and Ibaraki. Fig. 3 Compositions of PAHs in (a) Noge, (b) Kudan and (c) Tsukuba. Rehwagen et al., 2005) PAH NPAH (Kojima et al., 2010) PAH NPAH PAH NPAH PAH NPAH PM 2009 PM 2 Fig. 5 Variation of 1-NP / Pyr ratio in (a) Noge, (b) Kudan and (c) Tsukuba. PAH NPAH (Morikawa and Mizohata, 2013) PAH NO 2 CO (Fig. 4) 2012; 2014 PAH

5 NPAH PAH NPAH / PAH 2,500 1-NP / Pyr , (Tang et al., 2005) 3 1- NP / Pyr Fig. 5 PAH NPAH NP / Pyr , , NP / Pyr PAH NPAH NP / Pyr NO x NO 2 (Fig. 4) PAH PAH Pyr NO x 1-NP Pyr 1-NP / Pyr 7-NBaA / BaA 6-NBaP / BaP 1-NP / Pyr PAH NPAH 1-NP / Pyr NO x Ames, B. N., McCann, J., Yamasaki, E.: Method for detecting carcinogens and mutagens with the salmonella/mammalian-microsome mutagenicty test, Mutat. Res., 31, (1975). Atkinson, R., Arey, J.: Atmospheric chemistry of gas-phase polycyclic aromatic hydrocarbons: Formation of atmospheric mutagens, Environ. Health Perspect., 102, (1994). Epstein, S. S., Fujii, K., Asahina, S.: Carcinogenicity of a composite organic extract of urban particulate atmospheric pollutants following subcutaneous injection in infant mice, Environ. Res., 19, (1979) , 1 8 (2012). Hayakawa, K., Kitamura, R., Butoh, M., Imaizumi, N., Miyazaki, M.: Determination of diamino- and aminopyrenes by high performance liquid chromatography with chemiluminescenece detection, Anal. Sci., 7, (1991). Hayakawa, K., Butoh, M., Hirabayashi, Y., Miyazaki, M.: Determination of 1,3-, 1,6-, 1,8-dinitropyrenes and 1-nitropyrene in vehicle exhaust particulates, Jpn. J. Toxicol. Environ. Health., 40, (1994). Hayakawa, K., Kawaguchi, Y., Murahashi, M., Miyazaki, M.: Distributions of nitropyrenes and mutagenicity in airborne particulates collected with an Andersen sampler, Mutat. Res., 348, (1995). : environment/observation.html International Agency for Research on Cancer: Agents Classified by the IARC Monographs, Volumes 1 109, Kakimoto, H., Matsumoto, Y., Sakai, S., Kanoh, F., Arashidani, K., Tang, N., Akutsu, K., Nakajima, A., Awata, Y., Toriba, A., Kizu, R., Hayakawa, K.: Comparison of atmospheric polycyclic aromatic hydrocarbons and nitropolycyclic aromatic hydrocarbons in an industrialized city (Kitakyushu) and two commercial cities (Sapporo and Tokyo), Journal of Health Science, 48, (2002). Kojima, Y., Inazu, K., Hisamatsu, Y., Okochi, H., Baba, T., Nagoya, T.: Changes in concentration levels of polycyclic aromatic compounds associated with airborne particulate matter in downtown Tokyo after

6 122 J. Jpn. Soc. Atmos. Environ. Vol. 50 No introducing government diesel vehicle controls, Asian J. Atmos. Environ., 4-1, 1 8 (2010) Morikawa, T., Mizohata, A.: Source Apportionment Study of Atmospheric Particulate Matter at a Road Side and Ambient in Tokyo, from 2002 to 2012, JARI Research Journal (2013). Murahashi, T., Miyazaki, M., Kakizawa, R., Yamagishi, Y., Kitamura, M., Hayakawa, K.: Diurnal concentrations of 1,3-, 1,6-, 1,8-dinitropyrenes, 1-nitropyrene and benzo a pyrene in air in downtown Kanazawa and the contribution of diesel-engine vehicles, Jpn. J. Toxicol. Environ. Health., 41, (1995). Rehwagen, M., Muller, A., Massolo, L., Herbarth, O., Ronco, A.: Polycyclic aromatic hydrocarbons associated with particles in ambient air from urban and industrial areas, Sci. Total Environ., 348, (2005). Tang, N., Tabata, M., Mishukov, V. F., Sergienko, V., Toriba, A., Kizu, R., Hayakawa, K.: Comparison of atmospheric nitropolycyclic aromatic hydrocarbons in Vladivostok, Kanazawa and Toyama, Journal of Health Science, 48, (2002). Tang, N., Toriba, A., Kizu, R., Hayakawa, K.: Improvement of an automatic HPLC system for nitropolycyclic aromatic hydrocarbons: Removal of an interfering peak and increase in the number of analytes, Anal. Sci., 19, (2003). Tang, N., Hattori, T., Taga, R., Igarashi, K., Yang, X., Tamura, K., Kakimato, H., Mishukov V. F., Toriba, A., Kizu R., Hayakawa, K.: Polycyclic aromatic hydrocarbons and nitropolycyclic aromatic hydrocarbons in urban air particulates and their relationship to emission sources in the Pan-Japan Sea countries, Atmos. Environ., 39, (2005) /60o8q100.htm Toriba, A., Kuramae, Y., Chetiyanukornkul, T., Kizu, R., Makino, T., Nakazawa, H., Hayakawa, K.: Quantification of polycyclic aromatic hydrocarbons (PAHs) in human hair by HPLC with fluorescence detection: A biological monitoring method to evaluate the exposure to PAHs, Biomed. Chromatogr., 17, (2003) PAH/NPAH (PAH) 9 (NPAH) 3 HPLC- HPLC-PAH NPAH PAH NPAH 1-NP / Pyr PAH NPAH NO x

7 50 2 pp PAH/NPAH

研究成果報告書(一部基金分)

研究成果報告書(一部基金分) 13 PM SO 2 PAH PAH SO 2 PAH PAH NPAH PAH PAH PAH PAH 2014 2 21 5 29 (MP-Σ500N, SHIBATA) 5 L/min (55 mmφ T60A20 ) 2009 3 9 5 2 7 17 9 26 1 2 (HV1000R, SHIBATA) 2012 3 1 5 31 10 1 11 29 2013 3 1 5 30 (203