1 埼玉大学紀要工学部第 38 号 Deposition of air pollutants on airborne Cryptomeria japonica pollen in urban areas of Kanto Plain, Japan Qingyue WANG, Daisuke AOKI and Kazuhiko SAKAMOTO The morbidity due to Cryptomeria japonica pollinosis so-called Japanese Cedar Pollinosis is increasing, especially in the urban areas of Kanto Plain in Japan. The reasons of this increase might have been associated with airborne pollutants from the biomedical tests conducted on mice and rats. The overall purposes of this study were to investigate whether air pollutants may deposit onto airborne Cryptomeria japonica pollen or not during the pollen flying season, and thereby also try to find out the influence of airborne pollutants on the pollinosis, the results of which may advance the further biomedical researching. We investigated deposition of air pollutants on Cryptomeria japonica perigonium pollen and what pollutants may deposit together with the airborne pollen to respiratory tract between urban and mountainous areas. Metallic, ionic and carbonic components of suspended particulate matter (SPM) and perigonium pollen collected at the urban of Saitama City and the mountainous areas of Okuchichibu during the season were analyzed to identify their relationship. We found that crustal particles (Al, Fe and Ti) tended to deposit on the perigonium pollen. The amount of ionic components of anthropogenic secondary particles (NO - 3, SO and NH ) deposited on the perigonium pollen were higher in the urban than in the mountainous areas. It suggested that these airborne pollutants may affect the pollinosis, and it is important to determine airborne Cryptomeria japonica pollen and its major allergen (Cry j I), and investigate the chemical, physical and biomedical combination effects on it in our further study. Keywords: Cryptomeria japonica pollen, Perigonium, Suspended particulate matter (SPM), Ionic components, Metallic components, Carbonic components and Crustal particles 1. ), 5) 20 1) 2 3) 1), Department of Environmental Science and Human 6) Engineering, Graduate School of Science and Engineering, Saitama University, 255 Shimo-Okubo, Sakura-ku, Saitama City, Saitama , Japan

2 都市近郊農地としての見沼田圃の環境的価値に関する研究 82 7), 8) Cry j I 2. 9) 2.1 Cry j I /23/8 3/113/16 11), 12) AH-600, AHV 2 (Fig. 2 (a)) AHV (Fig. 1) L min (Dp: particle size)7 µm, 2 Dp3.37 µm, How about recent studies? Animal exposure 3 Dp23.3 µm, Dp1.12 µm, 5 Biomedical tests Questionnaire survey How about deposition of air pollutants? DEP, DEG, SPM, etc. VOC, SVOC NOx, SO 2, NH 3, HNO 3, etc. Secondary particles: NH NO 3, (NH ) 2 SO Humidity, etc. Pollen Cryptomeria japonica Pollen (Dp: ca. 30 mm) Allergen release Yubissu bodies (Dp 1 mm) Adjuvant effects Aeroallergens Cry j I, etc. Our studies Fig. 1 Concept of pollen-air pollutant possible interaction processes in our studies. Here, DEP: diesel exhaust particulates, DEG: diesel exhaust gases, SPM: suspended particulate matter, VOC: volatile organic carbon, SVOC: semi-volatile organic carbon, Cry j I: major allergen of the pollen and Dp: particle size. Dp 1.1 µm AHV 1~ (Dp >1.1 µm) ( AHQ-630) 5 (Dp <1.1 µm) 2500QAT-UP ( )

埼玉大学紀要工学部第 38 号 2005 83 DK-1SA Fig. 2 (b) ( Model GLB-B1500MBITaN) (SEM,, Model S-200) 1~ (Dp >1.1 µm) 18 1 12 5 (Dp <1.

2 (a)) 3 ml 3 3 ml 3 3 Weather vane Hygrothermograph Data carrier 100 30 3 ml 1 10 ml Slide glass (0) (Al, Ba, B, Ca, Cd, Cr, Cu, Fe, Li,

3 埼玉大学紀要工学部第 38 号 DK-1SA Fig. 2 (b) ( Model GLB-B1500MBITaN) (SEM,, Model S-200) 1~ (Dp >1.1 µm) (Dp <1.1 µm) 7 mmφ g 30 ml, EDOMET(Fig. 2 (a)) 3 ml 3 3 ml 3 3 Weather vane Hygrothermograph Data carrier ml 1 10 ml Slide glass (0) (Al, Ba, B, Ca, Cd, Cr, Cu, Fe, Li, Mg, Mo, (a) Andersen high volume air sampler (b) Pollen sampler (counter) Fig. 2 Sampling equipments used for collecting airborne particulate matter and pollen. Na, Ni, Pb, Sb, Ti, Zn, Sc, Sr, V) ICP-AES,, JICP-PS1000UV g 50 ml 10 2

4 都市近郊農地としての見沼田圃の環境的価値に関する研究 8 5 ml Dp < 2.0 µm 50 µl 0.27 M NO - 3,SO, NH Na 2 CO 3 /0.03 MNaHCO 3 2 ~ Al, Fe, Ti, DX-100 (F -, Cl -, 1 m s -1 NO 2 -, Br -, NO 3 -, PO 3-, SO, (COO) 2 - ), (Na, NH, K, Mg 2, Ca 2 ) (Organic Carbon : OC) (Elemental Carbon : EC) 8 mmφ 2.0 DRI, Model 2001 TOC(Total Organic Carbon, 120~550 ) TEC (Total Elemental Carbon, 550~800 ) Py-OC (Pyrolyzed OC) Dp: particle size (µm) Fig. 3 Size-distribution of the ionic concentrations 3.1 of airborne particles collected in mountainous and urban areas M (n= 7) 6.0 U (n= 6) Fig (NH, SO, NO - 3, Cl - ) Fig. 0.0 Al, Fe, Ti, NO - 3, SO, NH Al Fe Ti NO - 3 SO NH Fig. Al, Fe, Ti, NO - 3, SO, NH concentrations of airborne particles collected in mountainous (M: Okuchichibu) and urban (U: Saitama City) areas. The bars show the standard deviation. Concentration (µg m -3 ) Concentration µg m -3 ) Concentration µg m -3 ) (a) Urban areas Cl - SO NO 3 - NH (b) Mountainous areas Cl - SO NO 3 - NH

5 埼玉大学紀要工学部第 38 号 m s -1 Crustal particulate Al, Fe, Ti Table 1 Table 1 Al, Fe and Ti concentrations of Cryptomeria japonica periponium pollen collected in 100µm mountainous (M) and urban (U) areas. (b) Site Al Fe Ti (µg m -3 ) M: Okuchcibu (n = 8) n.d. a) n.d. a) n.d. a) Fig. 5 Scanning electron micrographs of pollen surfaces U: Saitama City (n = 8) 1,070 1,10 52 (a) suspended pollen and Kanto loam dust in the chamber experiment ), and Cryptomeria japonica a) n.d. means below the limit of detection. perigonium surfaces (b) collected in the urban area in this study. Al, Fe, Ti Al, Fe AlFeTi (a) 20 µm Crustal particulate 15) ( ) 13) AlFeTi AlFeTi Maejima 1) NO - 3,SO, NH Fig. 6 Fig. 3 Fig. 2 ~ Fig. 5(a) Fig. 6 (Fig. 5 (b)) NO - 3,SO, NH

6 都市近郊農地としての見沼田圃の環境的価値に関する研究 86 Concentration (µg g -1 ) M (n = 8) NO - 3 SO NH U (n = 8) Fig. 6 NO 3 -, SO, NH concentrations of Cryptomeria japonica periponium pollen collected in mountainous (M) and urban (U) areas. The bars show the standard deviation. NO - 3, SO, TEC TOC TOCA NH TEC TECTC (%)(TC = TEC TOC) TOCA NOx, SO 2, NH 3, HNO 3 EC NO - 3, SO, NH TOC TEC Fig. 3 NO - 3, SO, NH 2 ~ Dp < 2.0 µm Dp<2 µm (, Dp>7 Fig. 8) µm) (DEP) IgE 1) Fig. 7 Size-distribution of TEC concentrations of air samples collected in mountainous (M) and urban (U) areas. TEC is total elemental carbon. OC 0 NO - 16), 17) 3 SO NH Fig. 7 Fig. 8 Ratios of ionic concentrations ([Ion]x (Urban) ) in DEP samples collected in urban area to ionic concentrations ([Ion]x (mountainous) ) collected in (TEC) Dp <2 µm mountainous area. Ratio of urban to mountainous areas TEC concentration µg m -3 ) [Ion]x (Urban) [Ion]x (Mountainous) Urban area Mountainous area Dp: particle size (µm) Ionic components in SPM Ionic components in pollen

埼玉大学紀要工学部第 38 号 2005 87 NO - 3, SO, NH ) Na NH Ca 2 TOC TEC 12), Dp <1 µm 18) Fig. 10 Particulate (Dp>7 µm) concentrations of air samples collected in mountainous (M) and urban (U) areas.

7 埼玉大学紀要工学部第 38 号 NO - 3, SO, NH ) Na NH Ca 2 TOC TEC 12), Dp <1 µm 18) Fig. 10 Particulate (Dp>7 µm) concentrations of air samples collected in mountainous (M) and urban (U) areas. TOC is total organic carbon, and TEC is total elemental carbon. SEM Fig. 9(a)~(f) U (n = 6) Al, Fe Table 1 M (n = 7) Al Fe Cl - NO - 3 SO Na NH Ca 2 TOC TEC Particulate air pollutants (Dp7 µm) concentration of collected air samples (µg m -3 ) (b) (c) (d) (e) Al, Fe (a) Pollen flying (Dp:: ~30~ µm) Formation of small particles (Dp: 10~20 µm) Transmutation Transport processes Yubissu bodies with air pollutants (Dp 1 µm) Transubstantiation (Dp 1 µm) Fig. 9 Morphological changes of cedar pollen during airborne transport to or within the urban area. (Dp: particle sizes) (f ) ( Fe 2 O 3, Al 2 O 3, SiO 2 ) IgE 19) Al, Fe. NO - 3, SO, NH Dp>7 µm AHV 1 Dp>7 µm Fig. 10 Al, Fe

8 都市近郊農地としての見沼田圃の環境的価値に関する研究 88 of diesel-exhaust particulates for the production of IgE 19) antibody in mice, Journal of Allergy and Clinical Immunology, 77, , ) Takafuji S., Suzuki S., Koizumi K., Tadokoro K., Ikemori R., Muranaka M., Diesel-exhaust particulates inoculated by the intranasal route have an adjuvant activity for IgE production in mice, Journal of Allergy Cry j and Clinical Immunology, 79, , 1987 I 9),. 32, 9, ) Miki-Hiroshige, H., Nakamura, S., Yasueda, H., Shida, T., Takahashi, Y., Immunocytochemical localization of the allergenic proteins in the pollen of Cryptimeria japonica, Sex Plant Reprod 7, , ) Takahashi Y., Sakaguchi M., Inouye S., Miyazawa H., (B)No Imaoka K., Katagiri S., Existence of exine-free airborne allergen particles of Japanese cedar pollen. Allergy, 6, , ) Takahashi Y., Sasaki K., Nakamura S., Miki-Hiroshige H., Nitta H., Aerodynamic size distribution of the 1),,, 36, particles emitted from the flowers of allergologically 17-27, 1998 important plants, Grana, 3, 5-9, ) 13), ) Watanabe N., Ohsawa M., Elevated serum 9, , 199 immunoglobulin E to Cryptomeria japonica pollen in rats exposed to diesel exhaust during fetal and neonatal periods, BMC Pregnancy and Childbirth, 25, 1-9, ) Maejima, K. Tamura, K., Nakajima, T., Taniguchi, Y., Saito, S., Takenaka, H., Effects of the inhalationof diesel exhaust, Kanto loam dust, or diesel exhaust ),,,, without particles on immune responses in mice,,,,, exposed to Japanese cedar (Cryptomeria japonica) pollen, Inhalation Toxicology,13, , 2001,,, 15),,, 51, , ),,, 22, 3-38, ),,,, 22, , ) Muranaka M., Suzuki S., Koizumi K., Takafuji S., Miyamoto T., Ikemori R., Tokiwa H., Adjuvant activity 10 -, , ) Wang Q., Aoki D. and Sakamoto K., Basic Observation

9 埼玉大学紀要工学部第 38 号 on Interaction between Air Pollutants and Ingredient Matter Released from Various Pollens, The Paper of International Conference of Atmospheric Environment (October 2~26, Nanning, China), 23-22, ),,, 5 (10 20~22 ),, 2D0915, 536, ) Takahashi Y., Sakaguchi M., Inouye S., Miyazawa H., Imaoka K. and Katagiri S., Existence of exine-free airborne allergen particles of Japanese cedar (Cryptomeria japonica) pollen, Allergy, 6, , ) , 2000

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