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90 Stainless tube Outlet Heater Heater Stainless tube Vinyl chloride tube Temperature sensor Air pump (20L/min) Mimic measurement points (five points) Temperature sensor Temperature controller Temperature controller Stainless steel containerl Raw materialboron acid Drying ovenmax 220 Temperature sensor Washing device of the discharge gas Temperature controller Caustic soda Fig.1 The generator of boron compounds. Filter paper holder (25mmStainless steel) (0.2m Teflon filter ) Polypropylene bottle Heater Temperature sensor Temperature controller (130) Wet gas meter Vacuum pump 3%hydrogen peroxide Fig.2 Schematic illustration of boron measurement for the exhaust gas. (20L/min) Air pump Outdoor air Hot air generator Air pump (20L/min) Drying ovenmax 220 Temperature controller Sensor of temperature Raw materialboron acid Temperature controller Heater Sensor of temperature Measurement points Fan Heater Artificial environment control room (35) Boron compound exposure chamber Artificial environment control room (35) Non-boron compound exposure chamber cooler Fig.3 Schematic illustration of artificial exposure chamber. Temperature controller Outlet wet scrubber (Draft fan Measurement points Senser of temperature

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92 Fig.4 The damaged strawberry leaves by gas-phase boron compounds. (Exposed periods)

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94 Mass, mg/m Al, µg/m Ca, µg/m Sr, µg/m Na, µg/m Ni, µg/m H H H H H H H

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96 H15 H16 H17

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99 4-4-t- A SDBRPS 5mL 5mL ph3.5 10mL 500mLpH3.5 10mL2 1mol/L 0.5mL 0.2mL 10 1mol/L 4mL 3mL GC/MS 2g

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104 stn.e stn.a stn.b stn.c stn.d

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124 Daphnia magna Oryzias latipes

125 Vibrio fisheri

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128 Variation of ionic constituents in aerosol particles during kosa events in Toyama, Japan The th Asian Symposium on Ecotechnology ( August ) Mizuka KIDO8 Dynamics of dissolved organic matter in local area waters The First International Workshop on HAB in the Northwest Pacific Region ( June July) Hironori Fujishima

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130 SPM, TSP ug/m SPM TSP * * Concentrations, nmol/m nssca Na NO 3 - nssmg 2+ Sr Cl - nssso 4 2- NH 4 + April, 2003

131 Anion, % (Equiv.) Cation, % (Equiv.) 80 Cl April, 2003 NO 3 - SO 4 2- Na + NH 4 + K + Mg 2+ Ca 2+ Cl - +NO 3 - +SO4 2-, neq/m 3 NH 4 +, nmol/m 3 Cl -, nmol/m (a) Na + +NH 4 + +K + +Mg 2+ +Ca 2+, neq/m 3 sea water ratio (c) (b) 1:1 Na +, nmol/m :1 NO 3 -, nmol/m 3 nssmg 2+, nmol/m 3 Sr (ICP), nmol/m nssca 2+, nmol/m :2 1: (d) (e) (f) nssca 2+, nmol/m 3 1:1 nssmg 2+ /nssca 2+ =0.15 (r 2 =0.99) Sr/Ca= (r 2 =0.55) nssso 2-4, nmol/m 3 Ca (ICP), nmol/m 3

132 TSP, mg/m /4/ /4/28-5/2 2005/5/2-5/6 2005/5/6-5/9 Kosugi (10m a.s.l.) Tateyama (1,180m a.s.l.) Murodo, Tateyama (2,450m a.s.l.) 2005/5/9-5/ /5/13-5/ /5/16-5/20

133 SPM, TSP ug/m 3 Concentrations, nmol/m nssca nssso SPM TSP April, 2003 NO 3 - nssmg 2+ Na + Cl - NH 4 +

134 Fig.2 Kosa observation by the LIDAR and variation of SPM. concentration during Kosa observation. Fig.3 Backward Trajectories ending at 00 UTC 13 Mar 04 FNL Meteorological Data, by NOAA HYSPLIT Model. Kosa Air Pollution (Inversion Layer) Japan Sea Toyama Plain Kosugi 10m) Tateyama 1,180m) Mt. Tateyama (3,015m) 2,450m ) Tateyama Murodo Fig.1 Elevation of observatory at Kosugi, Tateyama and Tateyama Murodo.

135 Fig.4 Kosa observation by the LIDAR. Fig.5 Variation of Ox concentration. Fig.6 Temperature variation at Tateyama and Kosugi. Fig.7 Backward Trajectories ending at 03 UTC 05 Jun 04 FNL Meteorological Data, by NOAA HYSPLIT Model.

136 Strawberry (Mar.13-Epr.1) Eggplant (Epr.9-Epr.18) Lettuce (Epr.9-Epr.18) Salvia (May.6-May.22) Hydrangea (May.23-Jun.13) Mum (Jun.6-Jun.13) White oak (Mar.13-May.22) Coral ardisia (Epr.24-Jun.18) Conifer (Epr.24-July.11)

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140 Mass mg/m 3 nssca 2+ neq/m 3 Na + neq/m 3 nssso 4 2- NH 4 + neq/m 3 neq/m / / / / / /31-4/1 4/ / / /28-5/6 5/6-10 5/ / /17-21

141 nss-so4 2- NH4 20 (a) + Autumn (anthropogenic pulumes) NO3 - Cl - 15 Na + K + nss-ca Mg Total Fine Coarse nss-so4 2- NH4 20 (b) + Spring (non-kosa) NO3 - Cl - 15 Na + K + nss-ca Mg Total Fine Coarse nss-so4 2- NH4 20 (c) + Spring (Kosa) NO3 - Cl - 15 Na + K + nss-ca Mg Total Fine Coarse KH04-1KH02-3 JST RR2002 Concentrations of inorganic matters The concentration of (µg inorganic m -3 ) matters ( µg m -3 ) Concentrations of inorganic matters The concentration of inorganic matters ( µg m -3 ) (µg m -3 ) Concentrations of inorganic matters The concentration (µg of inorganic m -3 ) matters ( µg m -3 )

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148 (n=124) µ/ 3

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151 Sample filtrate (ph 2, 1M HCl) 200 ml, 1 ml/min Hydrophobic acids Hydrophilic nutrals DAX-8 Resin Hydrophilic 0.1 M NaOH Componentand 10mL, 0.3 ml/min Hydrophobic bases

152 a a. A B

153 Dynamics of dissolved organic matter in Toyama Bay, Hironori FUJISHIMA, Yukio SHINMURA, Yoshimitsu TOHEZO, Masato NAKAYAMA (Bulletin of Toyama Prefectural Environmental Science Research Center)

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155 SDB 47mm 5mL 5mL 5mL 5mL 10mL 10mL 500mL 500mL(pH3.6) 30% 5mL 10% 5mL 5mL 2 5mL 2 1mL 1mL HPLCUV 200ng GCMS

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173 Flow sensor Atomizer Emission Fog point Sampler Flow controller Fog generation point Atomizer Fan or Clean bench air intake point Fig.1 Leaching tests by artificial acid fog and pure water fog Air compressor Pomp Artificial acid rain or Pure water 47mmφ Exposure metal An acrylic ho Millipore filte (0.8µm,Whit AAWP,47mm

174 Table 2 Artficial acid rain Item Concentration Item Concentration ph NH µg/ml EC µs/cm Ca µg/ml SO µg/ml Mg µg/ml NO µg/ml Na µg/ml Cl µg/ml K µg/ml

175 2 (1)arbon stee plate. 1.5 Fe 1 Fe Days 4 (2)Bronze plate 3 Zn Zn 2 Zn (3)Aluminum alloy plate 0.8 Al 0.6 Al 0.4 Al (3)Aluminum alloy plate 0.15 Si Si 0.1 Si Days 20 (5)Lead plate 15 Pb Pb 10 Pb 5 0 Days Leaching amount of of Fe (mg) Leaching amount of Al (mg) Leaching amount of Si (mg) Leaching amount of Zn (mg) Leaching amount of Pb (mg) Days Days Leaching amount of Mg (mg) Leaching amount of Cu (mg) Leaching amount of Pb (mg) Leaching amount of Cu (mg) Fig.2 Accumulative variations of leaching amount. : Artificial acid fog + Aerosol + Gas : Pure water fog + Aerosol + Gas : Pure water fog + Gas (2)Bronze plate Cu Cu Cu Days (2)Bronze plate Pb Pb Pb Days (3)Aluminum alloy plate Mg Mg Days (4)Copper plate Cu Cu Cu Days

176 Table 3 Leaching contribution of various metal samples from artificial acid fog, gas and aerosol (Unit : %) Carbon steel Bronze Aluminum alloy Copper Lead Fe Cu Zn Pb Al Mg Si Cu Pb Artificial acid fog Aerosol Gas

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178 Carbon Condition steel Table 4 Average leaching amounts of various metal samples from artificial acid fog, gas and aerosol (Unit : µg/l) Bronze Aluminum alloy Copper Lead Fe Cu Zn Pb Al Mg Si Cu Pb 2001Average Average / Average Average / Average Average / : Artificial acid fog + Aerosol + Gas : Pure water fog + Aerosol + Gas : Pure water fog + Gas

179 Table 5. Concentration of ion species on the metals under condition (Artificial acid fog + Aerosol + Gas) (unit : mg/l) 2- SO 4 - NO 3 Cl - H + + NH 4 Ca 2+ Mg 2+ K + Na + Carbon Steel (A) BLANK(B) (A-B)/B*100 (%) t Bronze (A) BLANK(B) (A-B)/B*100 (%) t Aluminum Alloy (A) BLANK(B) (A-B)/B*100 (%) t Copper (A) BLANK(B) (A-B)/B*100 (%) t Lead (A) BLANK(B) (A-B)/B*100 (%) t : Significantt(0.05/2)=2.20(Significance test of difference between the two population means) BLANK(B) : Artificial acid fog + Aerosol + Gas Table 6. Concentration of ion species on the metals under condition (Pure water fog + Aerosol + Gas) (unit : mg/l) 2- SO 4 - NO 3 Cl - H + + NH 4 Ca 2+ Mg 2+ K + Na + Carbon Steel (A) BLANK(B) (A-B)/B*100 (%) t Bronze (A) BLANK(B) (A-B)/B*100 (%) t Aluminum Alloy (A) BLANK(B) (A-B)/B*100 (%) t Copper (A) BLANK(B) (A-B)/B*100 (%) t Lead (A) BLANK(B) (A-B)/B*100 (%) t : Significantt(0.05/2)=2.20(Significance test of difference between the two population means) BLANK(B) : Pure water fog + Aerosol + Gas

180 Wet depositions of H + (µg/ml) Wet depositions of H + (µg/ml) Wet depositions of H + (µg/ml) Table 7 Concentration of ion species on the metals under condition (Pure water fog + Gas) (unit : mg/l) 2- SO 4 - NO 3 Cl - H + + NH 4 Ca 2+ Mg 2+ K + Na + Carbon Steel (A) BLANK(B) (A-B)/B*100 (%) t Bronze (A) BLANK(B) (A-B)/B*100 (%) t Aluminum Alloy (A) BLANK(B) (A-B)/B*100 (%) t Copper (A) BLANK(B) (A-B)/B*100 (%) t Lead (A) BLANK(B) (A-B)/B*100 (%) t Days 0.2 Carbon steel Bronze Aluminum alloy 0.1 Copper Lead Carbon steel Bronze Alum inum alloy Copper Lead Days 0.05 Carbon steel Bronze Alum inum alloy Copper Lead Days Fig. 3-1 Variations of wet depositions of the H + under condition,and. : Significantt(0.05/2)=2.20(Significance test of difference between the two population means) BLANK(B) : Pure water fog + Gas Fig.3-1 Variations of wet depositions of the H + under condition, and condition Wet depositions of SO 4 2- (µg/ml) Wet depositions of SO 4 2- (µg/ml) Wet depositions of SO 4 2- (µg/ml) Carbon steel -5 Bronze Aluminum alloy Copper Lead Days 6 Carbon steel Bronze 3 Aluminum alloy Copper Lead Days Carbon steel -2.5 Bronze Aluminum alloy Copper Lead Days Fig. 3-2 Variations of wet depositions of the SO 4 2- under condition, and. Fig.3-2 Variations of wet depositions of the SO 4 2- under condition, and

181 Wet depositions of NO 3 - (µg/ml) Wet depositions of NO 3 - (µg/ml) Wet depositions of NO 3 - (µg/ml) Carbon steel -5 Bronze Aluminum alloy Copper Lead Days Carbon steel -0.5 Bronze Aluminum alloy Copper Lead Days Carbon steel -0.5 Bronze Aluminum alloy Copper Lead Days Days Fig. 3-3 Variations of wet depositions of the NO - 3 under condition,and. 2 Fig.3-3 Variations of wet depositions of the NO - 3 under condition, and Wet depositions of Ca 2+ (µg/ml) Wet depositions of Ca 2+ (µg/ml) Wet depositions of Ca 2+ (µg/ml) 1 0 Carbon steel -1 Bronze Aluminum alloy Copper Lead Days Carbon steel -0.1 Bronze Aluminum alloy Copper Lead Days Carbon steel Bronze -0.1 Aluminum alloy Copper Lead Days Fig.3-5 Variations of wet depositions of the Ca 2+ under condition, and Wet depositions of NH 4 + (µg/ml) Wet depositions of NH 4 + (µg/ml) Wet depositions of NH 4 + (µg/ml) Carbon steel -1 Bronze Aluminum alloy Copper Lead Days Carbon steel -0.5 Bronze Aluminum alloy Copper Lead Days Carbon steel -0.5 Bronze Aluminum alloy Copper Lead Days Days Fig. 3-4 Variations of wet depositions of the NH 4 + under condition,and. Fig.3-4 Variations of wet depositions of the NH 4 + under condition, and

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186 [Toyama Prefecture] Japan Sea Toyama Kosugi (10m) Tateyama (1,180m) Tateyama Murodo (2,450m) Fig.1 Location of Kosugi, Tateyama, Tateyama Murodo and Kosugi Washizuka. Kosugi Washizuka Kosa Air Pollution (Inversion Layer) Japan Sea Toyama Plain Kosugi 10m) Tateyama 1,180m) Mt. Tateyama (3,015m) 2,450m ) Tateyama Murodo Fig.2 Elevation of observatory at Kosugi, Tateyama and Tateyama Murodo.

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188 Fig.3-1 Kosa observation by the LIDAR. Fig.3-2 Kosa observation by the LIDAR and variation of SPM. concentration during Kosa observation.

189 Fig Backward Trajectories ending at 18 UTC 11 Mar 04 FNL Meteorological Data, by NOAA HYSPLIT Model. Table 1 The cases that Kosa observed. Date Time The height of Maximum SPM the air mass concentration confirmed by (g/m 3 ) LIDER (m) Observatory T.M. T. K. Fig Backward Trajectories ending at 00 UTC 13 Mar 04 FNL Meteorological Data, by NOAA HYSPLIT Model. The point of the source of Kosa flown in Toyama. Feb. 1, : Loess Plateau, Bardem Jilin. Feb. 14, : The Inner Mongolia, North China. Feb. 19, : Loess Plateau, The Inner Mongolia, Gobi. Feb. 20, : Gobi. Mar. 2, : North China., The Inner Mongolia, Gobi. Mar. 16, : Loess Plateau, Bardem Jilin. Mar. 31, : The Inner Mongolia, Gobi. Apr. 11, : The Inner Mongolia, North China. Apr. 16, : The Inner Mongolia, Loess Plateau Apr. 18, : Loess Plateau, The Inner Mongolia, Gobi. Apr. 22, : The Inner Mongolia, North China. Apr. 26, : The Inner Mongolia, Gobi, North China. May 6, : Loess Plateau, Gobi. May : Loess Plateau May : Loess Plateau, Bardem Jilin, Gobi. May : Loess Plateau T.M. : Tateyama Murodo T. : Tateyama K. : Kosugi

190 Fig.4-1 Newspaper account of Yellow layer appeared over Toyama plain in the daytime. Morning edition of the Kitanihon Shimbun, March 29, Fig.4-2 Kosa observation by the LIDAR.

191 Fig.4-3 Kosa observation by the LIDAR and variation of SPM. concentration during Kosa observation. Fig.4-5 Temperature variation at Tateyama and Kosugi. Fig.4-4 Backward Trajectories ending at 03 UTC 28 Mar 04 FNL Meteorological Data, by NOAA HYSPLIT Model. Fig.4-6 The vertical distribution of temperature in Toyama plain, in May 13, ).

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194 Fig.5-1 Kosa observation by the LIDAR. Fig Backward Trajectories ending at 03 UTC 18 Apr 04 FNL Meteorological Data, by NOAA HYSPLIT Model. Fig Backward Trajectories ending at 03 UTC 18 Apr 04 FNL Meteorological Data, by NOAA HYSPLIT Model. Fig Backward Trajectories ending at 09 Fig Backward Trajectories ending at 09 UTC 16 Apr 04 FNL Meteorological UTC 16 Apr 04 FNL Meteorological Data, by NOAA HYSPLIT Model. Data, by NOAA HYSPLIT Model. Fig.5-2 Kosa observation by the LIDAR and variation of SPM. concentration during Kosa observation. Fig.5-4 Variation of Ox concentration during Kosa observation. Fig.5-5 Temperature variation at Tateyama and Kosugi. Fig.5-7 Variation of NOx and HC concentration during Kosa observation.

195 Table 2 The cases that Kosa and oxidant of high concentration were observed at the same time. Date Time The height of the air Maximum SPM Maximum Ox The point of the source of Kosa and air pollutions(oxidant) flown in Toyama. mass confirmed by LIDER (m) concentration (g/m 3 ) concentration (ppb) Kosa Air P. Observatory Observatory Kosa Oxidant N.S.P. S.P. T.M. T. K. T.M. T. K. Feb. 1, : Loess Plateau, Bardem Jilin. Vladivostok, North-Korea, North China. Feb. 20, : Gobi. Korea- Soul, China- Shandong Province. Mar. 16, : Loess Plateau, Bardem Jilin. Kansai region, China- Jiangsu Province Apr. 11, : The Inner Mongolia, North China Kansai region, Chukyo region, China- Bohai Sea, China- Shandong Province Apr. 22, : The Inner Mongolia, North China Kansai region, Kita Kyushu region, China-Dalian, China- Jiangsu Province Apr. 26, : The Inner Mongolia, Gobi, North China China- Bohai Sea, China- Shandong Province May 6, : Loess Plateau, Gobi. Kansai region May 13, : Loess Plateau Kanto region May 21, : Loess Plateau China- Jiangsu Province, China- Zhejiang Province Air P. : Air Polussion N.S.P. : Non-spherical Particle S.P. : Spherical Particle T.M. : Tateyama Murodo T. : Tateyama K. : Kosugi

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197 Fig.6-1 Kosa observation by the LIDAR. Fig Backward Trajectories ending at 03 UTC 05 Jun 04 FNL Meteorological Data, by NOAA HYSPLIT Model. Fig.6-5 Variation of NOx and HC concentration. Fig.6-2 Variation of Ox concentration. Fig.6-3 Temperature variation at Tateyama and Kosugi. Fig Backward Trajectories ending at 09 UTC 05 Jun 04 FNL Meteorological Data, by NOAA HYSPLIT Model.

198 Table 3 The cases that oxidant of high concentration were observed. Date Time The height of the air mass confirmed by LIDER (m) Maximum SPM Maximum Ox concentration (g/m 3 ) concentration (ppb) Observatory Observatory T.M. T. K. T.M. T. K. The point of the source of air pollutions(oxidant) flown in Toyama. Mar. 10, : Kansai region. Mar. 24, : Kanto region, Chukyo region. May 2, : Kanto region. May 28, : Chukyo region. T.M. : Tateyama Murodo T. : Tateyama K. : Kosugi

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