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1 Investigation of the Characteristics and the Sources of Polycyclic Aromatic Hydrocarbons in the Atmosphere

2 Department of Environmental Engineering and Management, Chaoyang University of Technology Thesis for the Degree of Master Investigation of the Characteristics and the Sources of Polycyclic Aromatic Hydrocarbons in the Atmosphere (Hsi-Hsien Yang) (Chia-Mei Chen) 17, July 2003

3 (Polyclic Aromatic Hydrocarons, PAHs) PS-1 PAHs 21 PAHs (GC/MS) 20 PAHs (ISCST3) (Cluster analysis) (Chi-square test) (CMB) CMB (1) PAHs (2) ISCST3 PAHs PAHs PAHs (3) PAHs PAHs PAHs (4) CMB PAHs (5) CMB PAHs 36.5% 4.03% 47.9% 8.33% 3.21% (6) CMB 8.0 CMB PAHs CMB PAHs -I-

4 Abstract The characteristics and the sources of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere were investigated. Particulate and PAHs samples were collected by high volume samplers, micro-orifice uniform deposit impactor (MOUDI), dry deposition sampling devices and wet deposition sampling devices. Twenty-one PAHs were analyzed by a gas chromatography/mass spectrometer (GC/MS). ISCST3 model, cluster analysis, chi-square test and chemical mass balance (CMB) receptor model were used to identify and quantify the PAHs emission sources. The results of CMB modeling were validated by emission inventories and ground-based trajectories.the results of this study are as follows: (1) The concentration, dry deposition, wet deposition and the particle size distributions of the particulate matter and PAHs in the atmosphere of the central Taiwan were characterized in this study. (2) The results of ISCST3 model analysis showed that the contribution of PAHs from the municipal solid waste incinerator (MSWI) was insignificant for the seven sampling sites. However, the results of cluster analysis and chi-square test indicated the atmospheric PAHs profiles at these sampling sites were correlated to that of MSWI. (3) Seven low reactive PAHs did not provide good estimation for CMB model analysis. The reason could be that less species were chosen. (4) The validation of CMB model analysis for particulate phase PAHs was not well examined by ground-based trajectories. The results showed that total (gas + particulate) phase PAHs should be considered for CMB analysis. (5) CMB receptor model for PAHs showed that the apportionment of the sources are: mobile source 36.5%, heavy oil combustion 4.03%, natural gas combustion 47.9%, coal combustion 8.33% and diesel combustion 3.21% (6) The validation of CMB model analysis with emission inventories and ground-based trajectories showed that CMB could be used to apportion source emission of PAHs. -II-

5 -III-

6 ...I... II... III...IV...IX... XII PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs IV-

7 PAHs PAHs ISC ISC CMB VOCs PAHs CMB V-

8 PS PAHs PAHs VI-

9 4-6 PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs ISCST ISCST ISCST PAHs PAHs PAHs VII-

10 PAHs PAHs CMB PAHs CMB VIII-

11 -IX PAHs PAHs 25 C (Eπ) PAHs PAHs PAHs MOUDI PAHs GC/MS PAHs (Chem Service) PAHs (Gravimetric Certificate) PAHs 10 µg ml -1 GC/MS PAHs 10 µg ml -1 GC/MS PAHs PAHs GC/MS PAHs GC/MS PAHs PAHs PAHs

12 5-1-4 PAHs PAHs PAHs PAHs MMD o g, o PAHs MMD g ISCST3 PAHs PAHs PAHs PAHs PAHs PAHs PAHs X-

13 PAHs (%) PAHs (%) CMB PAHs CMB PAHs CMB PAHs CMB PAHs CMB PAHs XI-

14 2-1-1 Bap DNA PS PS PS MOUDI MOUDI Nap, AcPy, Acp Flu PA, Ant, FL Pyr CYC, BaA, CHR BbF BkF, BeP, BaP PER IND, DBA, BbC BghiP COR PAHs (a) (b) PAHs PAHs PAHs XII-

15 PAHs ISC PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs ( MSWI) CMB 20 PAHs CMB 8 PAHs XIII-

16 1-1 (Polycyclic Aromatic Hydrocarbons, PAHs) 30 PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs PAHs (Receptor model) (CMB) PAHs CMB 21 PAHs PAHs 20 PAHs (ISCST3) (Cluster analysis) -1-

17 (Chi-square test) (CMB) CMB 1-2 PS-1 PAHs 1. PAHs PAHs PAHs 2. PAHs PAHs PAHs PAHs PAHs 4. PAHs PAHs (MMD) ( g ) 5. ISCST PAHs (CMB) CMB -2-

18 2-1 PAHs PAHs 1775 Pott Pott, 1775 (Polycyclic Aromatic Hydro-carbons PAHs) PAHs 1930 PAH Dibenz(a,h)anthracene (DBA) 1933 Benzo(a)pyrene (BaP) Cook, PAHs PAHs Dipple, 1976 PAHs PAHs (Soot) BaP PAHs PAHs 82 Clean Air Act, Title 30 (Polycyclic Aromatic Hydrocarbons, PAHs) / PAHs PAHs 21 PAHs PAHs PAHs -3-

19 PAHs Benzo(a)anthracene Benzo(a)pyrene Chrysene Benzo(b)fluoranthene Benzo(k)fluoranthene Indeno(1,2,3,c-d)pyrene Dibenzo(a,h)anthracene Bezno(g,h,i)perylene 8 PAHs Menzie et al, 1992 PAHs PAHs PAHs 82 PAHs 333 PAHs 1896 Karcher, 1983; Zandere, 1985; USEPA, 1987 PAHs (gas phase vapor phase) (particle phase) PAHs ( 25 ) (Electrophilic reaction, Eπ) PAHs 10-2 ~ atm (Semi-Volatile Organic Compounds, SVOCs) 10-8 atm 230 PAHs SVOCs PAHs 2000 PAHs PAHs PAHs Eπ PAHs PAHs Bjørseth and Ramahl, 1985; Dias, 1987; Ebert, 1988; Li and Kamens,

20 PAHs ( o C) ( o C) Naphthalene Nap Acenaphthylene AcPy Acenaphthene Acp Fluorene Flu Phenanthrene PA Anthracene Ant Fluoranthene FL Pyrene Pyr Cyclopenta[c,d]pyrene CYC 228 N.A. N.A. Benz[a]anthracene BaA Chrysene CHR Benzo[b]fluoranthene BbF Benzo[k]fluoranthene BkF

21 PAHs ( ) ( o C) ( o C) Benz[e]pyrene BeP Benzo[a]pyrene BaP Perylene PER NR Indeno[1,2,3-cd]pyrene IND 276 N.A. 534 Dibenz[a,h]anthracene DBA Benzo[b]chrycene BbC N.A. Benzo[ghi]perylene BghiP Coronene COR N.A. -6-

22 2-1-2 PAHs 25 C (Eπ) PAHs (mmhg) (µg L -1 ) Nap AcPy N.A. N.A. Acp N.A. Flu N.A. PA Ant FL N.A. Pyr CYC N.A. N.A. N.A. BaA N.A CHR BbF N.A. 2.0 N.A. BkF N.A. N.A. N.A. BeP BaP N.A (20 C) PER N.A IND N.A. N.A. N.A. DBA N.A. N.A BbC N.A. N.A BghiP N.A COR N.A N.A. Eπ -7-

23 PAHs PAHs 10-6 mmhg PAHs PAHs (Condensation) (Adsorption) Brostroem and Loevblad, 1991 PAHs ( ) 10-6 mmhg 10 µm 2000 PAHs PAHs PAHs PAHs 25 Nap 31.7 mg L -1 CHR mg L -1 Babara and Kames, 1986 PAHs PAHs PAHs PAHs (Causative agent) (Automobile Exhaust Condensate, AEC) Katz (1980) 5 µm 70~90% Grimmer (1983) 4~7 PAHs PAHs PAHs (C + ) DNA (Complementary base pair) T-A G-C (Cross-linking) -8-

24 DNA Josephson, 1984 (Ames) (Salmonella/Microsome reversion assay) Hecht, 1988 PAHs PAHs BaA CHR BbF BkF Bep BaP IND DBA Bghip BaP P-450 BaP BaP-7,8-Arene Oxide epoxide hydrolase BaP-7,8-Dihydrodiol P-450 BaP-7,8-Dihydrodiol 9,10-Epoxide DNA BaP-7,8-Dihydrodiol 9,10-Epoxide I-Deoxyguanosine adduct Rathore, 1991 BaP PAHs Promutagens PAHs (Direct acting mutagens) Perera and Ahmed (1979) 1 ng BaP 5% Levin et al. (1985) PAHs BaP Laskin (1970) SO 2 BaP SO (International Agency for Research on Cancer, IARC) (USEPA) (National Academy of Sciences, NAS) PAHs NAS, 1983; IARC, 1987; -9-

25 USEPA, 1991 IARC PAHs 2 A B 3 2 B2 PAHs D (Not classifiable) 2-3 S (Sufficient evidence) L (Limited evidence) I (Inadequate evidence) No Bjørseth and Becher, 1986 PAHs PAHs Tuominen (1988) 2~3 PAHs (Nitro-PAHs) (Screening test) PAHs ( PMS) PAHs ( Nitro-PAHs Choloric-PAHs ) (Activation) Longwell, 1982 CYC epoxide PAHs Davis et al.,

26 2-1-1 Bap DNA -11-

27 PAHs PAHs IARC USEPA NAS Nap 0 AcPy 0 Acp Flu 3 D I PA 3 D 0 I Ant 3 D 0 L FL 3 D + No Pyr 3 D 0 No CYC + L BaA 2A B2 + S CHR 3 B2 0/+ L BbF 2B B2 S BkF 2B B2 S BeP 0/+ I BaP 2A B2 ++ S PER 3 0 I IND DBA 2A B2 S BbC BghiP D + I COR 3 0/+ I 1. IARC 2A 2B 3 2. B2 PAHs D 3. S L I No S -12-

28 2-1-4 PAHs (µg ml -1 ) PMS PMS PMS PMS Bap PA FL CYC CYC epoxde Longewll (1982) PAHs PAHs (Pyro1ysis) PAHs PAHs PAHs PAHs 2000 ( ) PAHs PAHs Tuominen, 1988 Wybranies and Jong (1996) Cracow, Poland PAHs Harrison Sisovic (Birmingham) Zagreb PAHs 88% BaP BaP PAHs Harrison -13-

29 et al., 1996; Sisovic and Fugas, 1997 Mi (1996) ( 40 km hr km hr km hr -1 ) ( ) PAHs PAHs (5210 µg L -1 ) PAHs (3720 µg L -1 ) (1997) PAHs PAHs (49200 µg L -1 ) PAHs (1810 µg L -1 ) (1999) PAHs 27.2 mg min mg min mg min mg min mg min mg min -1 (1995) PAHs 31 µg km -1 PAHs 19.6 µg km -1 (1994) PAHs 10 Sheu et a1. (1996) µm PAHs % (1998) PAHs 87.8% PAHs PAHs 91.8% Barfknecht (1983) PAHs 10 PAHs Maschet et al. (1986) PAHs FL Pyr COR ( ) PAHs PAHs -14-

30 (Smoky coal) Mumford et al., 1987 PAHs PAHs 3,000 µg m -3 PAHs BaP 60 µg m -3 Ramdahl et al., 1982 Greenberg (New Jersey) PAHs 98% BaP Greenberg et al., 1985; Harkov and Greenberg, 1985 Michael et al. (1998) 70% 20~30% Teschke et al. (1989) Berg et al., 1988; Lofroth et al., 1991 (1994) ( ) PAHs PAHs PAHs Bjørseth Bjørseth and Ramahl, 1983 PAHs 19 µg kg µg kg

31 1 µg kg -1 (1999) PAHs 4350 µg kg µg L µg Kw -1 h -1 (1998) PAHs (3.10 mg L -1 ) (27.0 mg L -1 ( ) PAHs PAHs Akio and Youki (1987) PAHs 1,700~3,000 Wey and Shi (1997) PAHs Bjørseth and Ramahl (1983) PAHs 17 mg kg mg kg -1 Li et al. (1994) PAHs PAHs 1782 µg Nm -3 PAHs 6 µg g -1 PAHs 92% (1640 µg m -3 ) Li et al. (1995) PE PAHs PAHs PAHs PAHs ( ) PAHs (Coke) PAHs PAHs Trenholm and Beck, g ton -1 (Sintering) PAHs PAHs Bjorseth and Ramahl, 1983 (1999) PAHs 2140 µg -16-

32 Nm -3 2 Nap (86.5%) 7 COR (0.013%) (1998) PAHs PAHs 77.0~3970 µg kg -1 BaP 1.87~15.5 µg kg -1 ( ) PAHs PAHs PAHs Hoffman et al., 1984; Hoffman et al., PAHs PAHs PAHs (Pyrolysis) (Carbonization) Edwards, PAHs Badger PAHs Badger and Spotswood (1960) BaP BaP PAHs -17-

33 Frenklach (1985) PAHs A i + H A i +H 2 A i + C 2 H 2 A i C 2 H 2 A i C 2 H 2 +C 2 H 2 A i+1 +H A i i (I = 0~ ) Crittendern and Long (1976) (Styrene) PAHs PAHs PAHs PAHs PAHs Bjørseth and Ramahl, 1983 PAHs (Dehydrogenation) (Polymerization) (Carbonization process) PAHs (200 ) PAHs -18-

34 2000 Chen et al. (1997) PAHs 69.1% PAHs 1 µm 2.5 µm PAHs 73.9% PAHs ( 93%) 10 µm PAHs PAHs (Sub-micron-sized soot particle) Baek et al., 1991 PAHs ( ) 10-6 mmhg 10 µm PAHs Langmuir Langmuir PAHs Yamasaki et al., 1982 Langmuir : log K y =log C g / (C p / TSP) =-a (1/ T+b) (2-1) K y = - C g / (C p / TSP) = C g = PAHs C p = PAHs TSP= T= A,B= C g -19-

35 PAHs 10-6 mmhg PAHs PAHs PAHs PAHs Beck et al., 1991; Brostroem and Loevblad, 1991; Rudolph and Neue, PAHs (Primary pollutants) (NO 2 -AR/PAH) PAHs 290~400 nm PAHs PAHs 2000 Mcdow (1994) PAHs (Methoxyphenols) (Hexadecare) PAHs BaA BaP Jang Mcdow (1997) BaA 9, 10-anthraquinone 9-xanthone vaillin BaA benzo[a]anthracene-7 12-dione phthalic acid phthalic anhydride 1, 2-benzenedicar-boxaldehyde Sanders (1993) 11 PAHs Anthracene Benzo(a)pyrene Fluoranthene -20-

36 PAHs PAHs PAHs PAHs / (Blow-off) PAHs PAHs PAHs Bidleman et al., 1986 PAHs / Vaeck et al., PAHs 2. PAHs 3. PAHs 4. PAHs ; PAHs PAHs (Aging prosecc) PAHs Vaeck et al., 1984 Thrane Mikalsen (1981) CHR 1% 25% PAHs Coutant (1988) PAHs PA Ant 30~90% 5 PAHs PAHs Coleinar (1997) 1991~1995 PAHs -21-

37 PAHs 20~150 ng m -3 PAHs Sheu et al. (1996) PAHs PAHs 0.32 cm s cm s -1 PAHs cm s -1 Aceves Grimalt (1993) PAHs PAHs Lee et al. (1995) PAHs 46.1% 18.7% 20.6% PAHs ( ) PAHs (1995) PAHs ng m -3 PAHs 54% 31% 10% 8.0% (Respirable particulate) PAHs PAHs (Cascade impactor) Vaeck (1979) Sierra Anderson PAHs PAHs 2.5 µm 20% PAHs Aceves Grimalt (1993) PAHs 1.5 µm PAHs Venkatarainan Fried1ander (1994) mode mode I -22-

38 mode II PAHs PAHs 85% PAHs 0.12 µm PAHs 0.05~0.12 µm (mode I) 0.5~1.0 µm (mode II) Allen (1997) Oxygenated PAH (OPAH) OPAH PAHs OPAH 168~208 OPAH ( 2 µm) ( 2 µm) 248 OPAH PAHs PAHs PAHs Davies et al., 1976; Eiceman et al., 1981; Colmsjo et al., 1986 PAHs PAHs PAHs PAHs PAHs Hangebrauck (1967) PAHs 95% 87% Davies (1976) PAHs FL Pyr BaA + CHR BeP + BaP IND COR < 10 < 20 µg kg -1 PAHs < 0.01 < 0.01 µg kg -1 Huynh -23-

39 (1984) 70% PAHs 25% Morselli (1989) PAHs AcPy Flu CHR BkF BaP µg kg -1 (1997) PAHs 0.03% ~ 8.96% 2.28% PAHs Rantanen (1993) ( 50 ppm 20% 49) 56% 74% Westerholm (1986) 70% PAHs 30% PAHs PAHs PAHs PAHs PAHs PAHs PAHs -24-

40 1999 PAHs PAHs 2. PAHs PAHs ( ) PAHs (Dry Deposition) ( ) PAHs PAHs 2. (Wet Deposition) : (1) (rainout) (interception) (impaction) 1 µm (2) (washout) -25-

41 1 µm 2-2 (Nonprecipitation) Wu et al., 1992 (Eddy diffusion) Noll et al., (Aerodynamic transport) (Viscous sublayer) (Boundary layer transport) (Bounce-off) (Resuspension) 1/Vd = Ra + Rb + Rc (2-2) Ra = (Aerodynamic resistance) Rb = (Boundary layer resistance) Rc = (Surface resistance) -26-

42 Hicks (1986) (Suface analysis) (Atmospheric Flux) (Surrogate suface) (Through-Fall) (Foliar Extraction) (Vertical gradient method) (Eddy correlation method) (Variance method) Davison (1985),

43 Holsen et al. (1992) Lin et al. (1993) Sehmel (1980) µm (Brownian diffusion) (Eddy diffusion) 0.1 µm (Diffusion) -28-

44 Wu (1992) Vandberg Knoerr (1985) ( ) Davidson (1985) Noll (1988) 65%

45 (1994) Wu (1992) Holsen Noll (1992) Mylar 8 mg (Apiezon L Grease) 8 µm (1995) 20 mg (silicon grease) (1994) Ibrahim (1983) 7.5 µm 0.7 µm 15 Milford Dacidson (1987) (Mass Median Diameter, MMD) Nicholson (1988) Coe and Lindberg, 1987; Noll et al., 1988, 1990 Sehmel (1980) Davies Nicholson (1982) Sehmel Hodgson -30-

46 (1987) Gould Dacidson (1992) Wesely (1977) Ibrahim (1983) 40% Sehmel Hodgson (1987) Hillamo (1993) 0% 99% Z : Vd = F C ( z) (2-3) Vd F C (z) Z (Downward flux) (Resistance) -31-

47 Ra Rb Rc Vd = 1 Ra + Rb + Rc (2-4) Ra Rb Rc (mg m -2 day -1 ) (µg m -3 ) 1~15 10~15 cm/s 0.001~180 Sehmel, ~20 µm 20 µm Sehmel (1980) 0.1 µm 0.1~1 µm 1 µm Noll et al., 1990; Holsen et al., 1992; Ottley et al., 1993 Mcveety Hites (1998) PAHs cm s -1 PAHs 0.13~1.1 cm s -1 PAHs ( 2.5µm ) ( 0.1 µm 2.5 µm ) ( 0.1 µm) -32-

48 Holsen and Noll, 1992 Ligocki et al. (1985) PAHs (Washout) PAHs Mcveety Hites (1988) PAHs Siskiwit PAHs 9 Sheu et al. (1996) PAHs PAHs 0.31~3.2 µm PAHs (1998) PAHs 1.88% PAHs Nap AcPy 27.0% 36.5% PAHs 3.05% 95% 2-3 Lee et a1., 1993 ( ) -33-

49 Van Noort (1985) (In-cloud) (Below-cloud) (Diffusion) (Interception) (Impaction) ( ) Franz, 1998 Lee et al. (1993) Slinn et al.,

50 µm 1992 (1) (2) (3) -35-

51 Lovett and Kinsman, 1990 ( ) Horstmann and Mclachlan, PAHs PAHs (Henry s low constant) Slinn et a1., 1978; Eisenreich et al., 1981 Butler (1981) PAHs -36-

52 PAHs PAHs Paul et al., 1985 PAHs PAHs PAHs Van Noort, 1985; Bidleman, (Air-water coefficient) PAHs 2~4 PAHs Franz, 1998 (1998) PAHs PAHs PAHs 73% PAHs 27% Khemani (1985) Koelmans (1997) (Hydrophobic organic compounds) -37-

53 (Partition coefficient) PAHs ( ) 1996 PAHs PCBs 0.5 µm 0.5 µm 1999 Slinn (1978) ( ) / H(T) (atm m -3 mol) C v,atm (ng m -3 ) : C v,atm = 10 3 Cr H(T) / R T (2-5) (Washout) (2-6) (2-7) Slinn et al., 1978; Dickhut and Gustafson, 1995 W g = C d,rain / C v,atm (2-6) -38-

54 W p = C p,rain / C p,atm (2-7) C d,rain = (ng L -1 ) C p,rain = (ng L -1 ) W p = [(ng L -1 ) precipitation / (ng L -1 )air] Poster (1996) PAHs PAHs (< 0.05 µm) 0.05~1 µm S1inn et al., 1978; Wang, ~10 µm 0.5 µm (WD, F) [C p,r > 0.5 µm] / [ C p,air > 0.5 µm] (WD, nf) [C p,air < 0.5 µm] / [ C p,air < 0.5 µm] C p,air < 0.5 µm S1inn et al., 1978; PAHs MaCkay and Paterson,

55 PAHs PAHs (Soot carbon) PAHs PAHs 1996 (1) (2) (3) PAHs Readman, 1984; Boulzubassi, 1991; Brornan, 1991 ( PAHs) Poster and Baker (1996) (W g ) [C d ] / [C g ] [C d ] [C g W p [C p ] / [C p, air ] [C p ] [C p, air ] [C p, air ] / [C g + C p, air ] W p Bidleman, 1988 W g Ligocki et al.,

56 PAHs (Nucleation) (Coagulation) (Adsorption) (1) (2) (3) (4) (5) (1) (2) (3) (4) Perera, : (1) 0.1 µm (2) 0.1~2 µm 1 (3) 2 µm Frederica,

57 µ Frederica,

58 5 µm 5 µm 2 µm (TSP) ( PM 10 ) (Respirable suspended particulate PM 2.5 ) 2.5 µm 2.5 µm Watson et al., 1998a (Coarse mode) (Accumulation mode) (Nucleation mode) Watson et al., 1998a; Lundgren and Burton, µm 0.08 µm ~ 2 µm 2 ~ 3 µm -43-

59 Lundgren and Burton, 1995 PM 10 PM ~ Hi-vol PM 10 Dichotomous PM 10 PM % ~ 60.6% PM 10 PM ~ 5.6 µm 0.56 ~ 1.0 µm 1999 ( ) SO 2-4 NO - 3 NH Li and Okada (1999) 100 km (0.2 ~ 4 µm) Pierce Katz (1975) Toronto PAHs -44-

60 5 µm 85~90% 70~85% Vaeck (1979) 85~90% 90~95% PAHs Aceves (1993) 0.5 µm PAHs 1.5 PAHs (MW 202) Venkataraman Friedlander (1994) PAHs PAHs 85% PAHs 0.12 µm 0.5~1.0 µm PAHs 0.05~4.0 µm 0.05~0.12 µm (model I) 0.5~1.0 µm (model ) Model I model Accumulative mode (1995) PAHs 1.0 µm 1.0 µm (1996) PAHs PAHs 5.6~10 µm 0.31~0.52 µm 0.31~3.2 µm 0.52~1.0 µm (Cumulative distribution) MMD (Mass median of diameter) g -45-

61 (Geometric standard deviation) 2.5 µm ( 2.5 µm) ( 2.5 µm) (Mass median diamneter, MMD) 50% Pierce Katz (1975) CHR BaA BaP BkF PER BghiP Ant COR PAHs MMD 2.0~2.8 µm 1.2~1.6 µm PAHs Katz Chen (1980) Hamilton PAHs BghiP BaP BeP BkF MMD µm (1995) PAHs MMD µm (1996) PAHs MMD µm PAHs MMED (Mass mean equivalent diameter) TSP PAHs (Aging process) Vaeck et al., 1979; Vaeck, ISC (Industrial source complex, ISC) U.S. EPA 1970 (Steady-state) ( ) ISC ISCST3 (Industrial source complex -46-

62 short-term) (U.S. EPA, 1995) ISC ( ) ( ) ISCST3 ISCST3 1. (Control pathway) ( ) ( ) 2. (Source pathway) UTM (m) (g s -1 ) (m) (K) (m s -1 ) 3. (Receptor pathway) UTM (m) 4. (Meteorology pathway) -47-

63 5. (Output pathway) (1) (2) Overall (3) ISC ISCST3 (Downwash) x y x z x y -48-

64 C ( x, y) = QKVD 2πu σ σ s y z y exp 0.5 σ y 2 (2-8) : C (x, y) (x (m), y (m)) Q ( / ) K ( Q g s -1 µg m -3 ) V ( ) D σ y σ z (m) u s (m s -1 ) (2-8) ( 0.1 µm) ISC (1992) ISC -49-

65 (1994) ISC SO 2 Pasquill ISC (1999) 1997 ISC3 MESOPUFFII SO 2 (1999) ISC PM 10 PM 10 PM 10 (2000) ISC CMB (2000) PM 10 ISC PM 10 (2000) ISC (2000) ISC Hao et al. (2000) ISCST3-50-

66 Lorber et al. (2000) ISCST3 10 Basham and Whitwell (2000) ISCST3 Honaganahalli and Seiber (2000) Salinas Valley ISCST3 CAMET ISCST3 0.7 CALPUFF Ma et al. (2002) ISCST3 8 km 8 km (Source model) (Receptor model) (Dispersion model) (Emission strength) -51-

67 (Finger print) Friedlander (1973) Hopke, 1991 U.S. EPA, 1984; U.S. EPA, 1990 Eulerian Langrangian

68 (Tracer) ~30% (Chemical mass balance, CMB) Belsley et al., 1980 (Multivariate receptor model) (Principal component analysis) (Factor (Multiple linear regression) CMB CMB 1972 Miller Friedlander Hidy (Chemical element balance CEB) Hopke, Cooper Waston (CMB) -53-

69 Cheng, 2001 C i = p j= 1 α F ij ij S j (2-9) C i i α ij i F ij j i S j j i j α 1 (2-9) C i (2-10) S j C i = p j= 1 F ij S j (2-10) CMB C = F S (2-11) C = n 1 n F = n p p S = p 1 p -54-

70 (Tracer property solution) (Linear least-square fitting) Watson, 1984 Waston Watson, (Composition) CMB Glover (1991) CMB (Granite City) PM 10 CMB (Source profile) Sharma Patial (1994) Chow (1992) (San Joaquin Valley) PM 10 Bakerfield (54%) -55-

71 (15%) (10%) (8%) 4% Waston (1994) Chow (1995) (San Joaquin) PM 10 45% 15~20% 5% Vega (1997) CMB PM 2.5 PM % 38% Chen (1997) ( 2.5 µm) ( 2.5 µm ) CMB VOCs (Volatial organic compounds, VOCs) VOCs Carter, VOCs Seinfeld (1991) VOCs ( ) VOCs 2~4-56-

72 VOCs VOCs NMHC 33% 31% 15% 1% 8% 1998 VOCs CMB CMB 8.0 Watson, 1998b Fujita, 1998 Fujita et al. (1997) CMB VOCs CMB 6.6~10 Fujita et al. (1998) CMB VOCs VOCs 60~70% 10~13.5 % 2~19% 3~10% 1% VOCs VOCs 3.9~7.9 2~4 Conner et al. (1995) Lin and Milford (1994) Lewis et al. (1998) 1990 Canister VOCs CMB ( ) Lin and Milford (1994) 2 61~65 % 4~8.2% Conner Lewis VOCs Conner 20~30% Conner CMB ( -57-

73 MOBILE ) NMOC 10% 30% NMOC 10% 20% CMB (1993) VOCs VOCs 54~72% 30~35% 7~10% (1999) TO VOCs CMB CMB 8.0 VOCs ( ) 47~68% 8~22% 6~20% 0.1~3% 6~21% VOCs PAHs 20 CMB µg m -3 Friedlander, ng m -3 Dzubay et al., Gordon, 1988; Daisey et al.,

74 PAHs Gordon and Bryan, 1973; Daisey et al., 1979; Daisey and Lioy, 1981 PAHs Daisey et al., 1979; Miguel and Pereria, 1989; Pistikopoulos et al., 1990; Li and Kamens, 1993 PAHs CMB Miguel and Pereria, 1989; Pistikopoulos et al., 1990; Li and Kamens, 1993 Daisey (1979) PAHs PAHs Gordon and Bryan, 1973 PAHs Rogge et al., 1991 Peters (1981) PAHs PAHs PAHs PAHs PAHs PAHs CMB PAHs Mastclet et al., 1986 Pitts et al. (1978) PAHs CMB CMB CMB PAHs -59-

75 Kamens et al., 1985, 1988 PAHs PAHs (Depletion) Masclet et al., (Gaseous oxidizing agents ) (Luminosity) PAHs 4. PAHs PAHs 5. PAHs 6. Nikolaou et al., 1984 PAHs Pistikopoulos (1990) PAHs (Relative decay index, RDI) Fluoranthene ( ) PAHs Fluoranthene (Decay factor) CMB PAHs ( ) PAHs PAHs Cheng Richard (1993) (Smog chamber) PAHs CMB PAHs -60-

76 CMB 66~85% 32~58% 22~69% PAHs PAHs CMB PAHs PAHs PAHs Masclet (1986) RDI RDI R PAH R Fla R Fla R Fla 1 RDI RDI ( 21~32 ) BaP DiBah Ant BghiPe InP COR BaA Ant BkF CHR BeP Pyr Fla RDI Bap Ant DiBahAnt BaA BeP Pyr BkF BbF Katz et al., 1979 Bap BghiPe BaA Pyr BeP CHR Fla COR Butler and Crossley, 1981 Venkatarman Friedlander (1994) CMB PAHs CMB PAHs PAHs BkF BkF BkF CMB PAHs PAHs PAHs PAHs BaA BaP BghiP DBA BbF CHR Pyr Flu InP BkF RDI COR PAHs PAH PAHs (FL Pyr BaA CHR BbF BkF BeP COR) -61-

77 PAHs D 1 b PAHs RDI a RDI f RDF e Masclet et al. (1986) D 2 c Pico Rivera Pistikopouls et al. (1990) Upland D 3 d Venkataraman et al. (1994) Winter Summer NaP AcPy AcP Flu Phen Ant 1,5 1, ,0 - - FL Pyr 1,5 1, ,7 - - CYC BaA 2, CHR 0,9 1, ,0 - - BbF 1,2 1, ,0 1 1 BkF BeP 1,3 1, ,7 - - BaP 3 3, PER IND 1,4 1, , DBA BbC Bghip 1,8 1, , COR a: RDI= Relative Decay RDI=R PAH /R Fla (Fla FL) R=C M /C m (C M C m ) b: 1 ~ 5 c: 8 ~ 11 d: 21 ~ 32 e: RDF=Relative decay factors = i / BkF = i=(1+k i ) -1 f: RDI=Relative decay index -62-

78 PAHs CMB ( ) PAHs CMB CMB Winchester and Nifong (1971) Hidy and Friedlander (1972) Kneip et al. (1973) Friedlander (1973) CMB CMB (Oregon Graduate Center) FORTRAN IV PRIME 300 CMB Watson, 1979 PRIME MB 64 KB CMB 1 6 CMB 7 C FORTRAN 10 MB 640 KB CMB 8.0 CMB 7 DOS MS Windows US EPA, 2001 CMB 8.0 PAHs PAHs CMB C = F S C F S ng/g -63-

79 C (ng m -3 ) = F (ng g -1 ) S (g m -3 ) CMB 1 7 CMB 8.0 VOCs VOCs CMB 8.0 CMB 8.0 VOCs (2002) CMB VOCs CMB 8.0 VOCs VOCs PAHs PAHs PAH PAH (%) F ij = [PAH i ] / [[PAH total ] Miguel et al., 1989; Pistikopouls et al., 1990; Cheng and Richard, 1993 Li and Kamens, 1993 CMB 8.0 j PAHs ( BkF) F ij = [PAH i ] / [BkF] PAHs Venkataraman and Friedlander,

80 Super highway ~ (A~G) PAHs A B D C E F G 900 tons m de-nox 0.5 km (site B) ~8 km (site F) (6~9 m) N B MSW A incinerator E C G F Km

81 3-1-2 PAHs PAHs PAHs 2001/7/9~7/10 A C D E F G 7/2~7/4 A B C D G 7/3~7/4 E F 7/2~8/1 A B C D ( ) 8/2~9/3 E F G 7/9~7/11 D 7/3 PAHs 10/11~10/12 C E G 10/3~10/5 A B C D E F G ( ) 9/3~10/2 A B C D 10/2~11/2 E F G PAHs 12/24~12/25 E F G 12/10~12/12 A B C D E F G ( ) 12/10~1/21 A B C D E F G 12/24~12/25 D G PAHs 2002/3/11~3/12 A B C D 3/12~3/14 A B C D E F G ( ) 3/4~4/2 A B C D E F G -66-

82 3-2 PS-1 (High volume air sampler) (Mirco-orifice uniform deposit impactor, MOUDI) PS-1 PAHs PAHs MOUDI PAHs PAHs PS-1 MOUDI PS-1 PAHs PAHs PAHs PAHs PS-1 1. General Metal Work Co. GPS1 PUF Sampler PAHs PAHs ( ) XAD-16 PAHs (1) (Dual chamber sampling module) (2) (Flow venturi) (3) (Magnehelic gage) -67-

83 (4) (Voltage variator) (5) (Elapsed time indicator) (6) (Blower motor) (7) (Timer) (8) (Exhaust hose) (9) (Aluminum shelter) PS-1-68-

84 2. Whatman International Ltd cm 0.8 µm PAHs 450 C PAHs 8 3. PAHs 20 mm 30 mm XAD mm ( ) PAHs XAD-16 XAD-16 (Soxhlet extractor) 1000 ml 4. PAHs PS-1 PAHs PAHs -69-

85 GMW High Volume Air Samplers (GMW Inc. ) GPS1 General Metal Works Inc. GMW-25 (GMW-25 calibration kit) (1) GPS1 (2) GMW-25 (3) (4) (5)

86 (6) (7) 5 6 ( 3-2-3) General Metal Works Inc. ( 3-2-4) GPS1-71-

87 3-2-3 PS PS-1-72-

88 MSP MOUDI Model No. 100 MOUDI (Cascade impactor) (Rotator) 9 (Stages) (Cutsize) ( 300 ) MOUDI 30 L min -1 (Impaction) MOUDI -73-

89 3-2-5 MOUDI MOUDI (µm) ( ) Stage 1 18 ~ 10 Stage 2 10 ~ 5.6 Stage ~ 3.2 Stage ~ 1.8 Stage ~ 1.0 Stage ~ Stage ~ 0.33 Stage ~ Stage ~

90 2. MOUDI MSP (Aluminum foil 37 mm) Gelman Sciences Zefluor ( 37 mm 2 µm) (Afterfilter) % C MOUDI SHINAGAWA SEIKI Model DC-5A (Dry gas meter) 10 L MOUDI 30 L/min 20 (1) MOUDI (2) (3)

91 (4) 3 ( 3-2-6) L min (sec) y = 1.95x R 2 = ( ) MOUDI -76-

92 (PVC) 21.6 cm 8.0 cm 0.8 cm ( 10 ) 10 cm cm 50 cm cm ( 3-2-8) % C cm 8 3. PAHs PAHs PAHs V d,tm = K (F t,tm ) / (C tsp ) (3-1) -77-

93 V d,tm = PAHs (cm s -1 ) K = F t,tm = PAHs (mg m -2 day -1 ) C tsp = PAHs (µg m -3 ) 50 cm 150 cm

94 8 cm 0.65 cm 5.5 cm 10 cm 8.0 cm

95 cm 30 cm 2 8 cm 3 cm 3 cm PAHs 2. PAHs (MFS A045F047A 0.45 µm 47 mm) PAHs % 24 ( Sartorius BP 211D 0.01 mg) (25 )

96 Graseby Anderson Auto5 TM (Auto5 TM Automatic Stack Sampler) Universal Analyzers Inc. (Sample cooler Model 1090) Auto5 TM PAHs Auto5 TM Universal Analyzers Inc. 4 C PAHs (Probe) PAHs (1) (Coaxial dust collection tube) 4 mm ~ 14 mm (Nozzle) T (Thermocouple) (Compensation wire) 1300 mm (2) (Model-1090, Universal Analyzers Inc.) (Stainless steel heat exchanger drainer) -81-

97 4~5 C PAHs (3) PAHs PAHs (Cartridge) 20 mm 30 mm XAD mm PAHs (Breakthrough test) PAHs (4) (Total pressure) (Static pressure) (Main body) (Z80-CPU) (Coefficient of pilot tube) 30 L min

98 (5) 0.6 (Teflon) (1) (a) PAHs 20 mm 30 mm XAD mm PAHs 8 ( XAD-16) Anderson g cm -3 XAD-16 AMBERLITE 800 m 2 g -1 62~70% XAD-16 (Soxhlet extractor) 1000 ml (b) PAHs 50% -83-

99 (2) PAHs PAHs PAHs ( PUF XAD-16 ) PAHs (3) ( 1 1) PAHs QA/AC / ( 6 4) PAHs PAHs 2 ml 3-3 PAHs PAHs PAHs 1. PAHs ( 16 cm 4 cm) 300 ml 250 ml ( 1 1)

100 PAHs PAHs ( ) ( 20 cm 7 cm) 800 ml ( 1 1) 24 4 ( 1 1) PAHs QA/AC / ( 6 4) PAHs PAHs 2 ml ml l ( 1 1) 100 m 5 10 cm ml ml

101 (Silica gel) 17 g 1 g 105 C 8 15 g 3% 400 C 24 2 ml 25 ml PAHs 10 ml 200 ml ml GC/MS PAHs 5. PAHs Agilent 6890/5973N (Gas Chromatograph / Mass Spectrometer, GC/MS) Agilent µl Agilent Ultra mm 0.17 µm 50 m C 20 C min

102 100 C 3 C min C 40 GC/MS 310 C (Ion source) 310 C -87-

103 PAHs (Reagent Blank) 250 ml 0.5 ml GC/MS 21 PAHs (IDL) (Field Blank) (Trip Blank) -88-

104 4-1-4 ( ) (1998) PAHs 25.3% PAHs 6% PAHs 4.5% PAHs PAHs 3 cm XAD-16 PAHs (Breakthrough test) XAD-16 ( ) XAD-16 PAHs

105 6.3 cm PUF XAD-16 resin PUF XAD-16 resin PUF 3 cm 2 cm 1 cm 2 cm 2 cm

106 PAHs PAHs XAD-16 PAHs (ng Nm -3 (%) ) N.D. XAD-16 PAHs (ng Nm -3 (%) ) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND N.D DBA N.D BbC BghiP COR

107 (2 cm ) XAD-16 PAHs 99.8% XAD-16 PAHs 0.208% 3 cm XAD-16 PAHs 99.8% 4-3 (Method Detection Limit, MDL) 99% (Confidence) MDL MDL MDL PAHs PAHs MDL Long Winefordner Long and Winefordner, 1983 MDL = 3 (S b 2 + S i 2 +(i/m) 2 S m 2 ) 1/2 /m (4-1) S b S i S m i m PAHs GC/MS MDL ~ ng GC/MS Nap BaA ~ 1.28 ng m

108 PAHs GC/MS MDL (ng) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR (ng m -3 ) -93-

109 4-4 (Calibration curve) ( ) (Least square srror equation) r 6. r ± 20%

110 4. 21 PAHs GC/MS ~ ( ) 10 µg ml -1 GC/MS (RSD) (Accuracy) (Precision) PAHs GC/MS GC/MS PAHs (X) X n= X + X +... X n 1 2 n (4-2) Χn Χ(%) = 100% (4-3) C X i n Xn C (RSD) n S 2 = [ ( X i Xn ) ] n 1 i= 1 S RSD(%) = X 100 n 1 2 (4-4) (4-5) -95-

111 2.5e+7 2.5e+7 Integrated Area 2.0e+7 1.5e+7 1.0e+7 5.0e+6 Nap R 2 = e+7 1.5e+7 1.0e+7 5.0e+6 AcPy R 2 = The Mass Injected to the GC/MS(ng) 2.5e+7 3.0e+7 Integrated Area 2.0e+7 1.5e+7 1.0e+7 Acp R 2 = e+7 2.0e+7 1.5e+7 1.0e+7 Flu R 2 = e+6 5.0e The Mass Injected to the GC/MS(ng) Nap, AcPy, Acp Flu -96-

112 2.5e+7 2.5e+7 Integrated Area 2.0e+7 1.5e+7 1.0e+7 5.0e+6 PA R 2 = e+7 1.5e+7 1.0e+7 5.0e+6 Ant R 2 = The Mass Injected to the GC/MS(ng) Integrated Area 2.5e+7 2.0e+7 1.5e+7 1.0e+7 5.0e+6 FL R 2 = e+7 2.0e+7 1.5e+7 1.0e+7 5.0e+6 Pyr R 2 = The Mass Injected to the GC/MS(ng) PA, Ant, FL Pyr -97-

113 Integrated Area 3.5e+6 3.0e+6 2.5e+6 2.0e+6 1.5e+6 1.0e+6 CYC R 2 = e+7 2.0e+7 1.5e+7 1.0e+7 BaA R 2 = e+5 5.0e The Mass Injected to the GC/MS(ng) Integrated Area 2.5e+7 2.0e+7 1.5e+7 1.0e+7 5.0e+6 CHR R 2 = e+7 2.0e+7 1.5e+7 1.0e+7 5.0e+6 BbF R 2 = The Mass Injected to the GC/MS(ng) CYC, BaA, CHR BbF -98-

114 Integrated Area 3.0e+7 2.5e+7 2.0e+7 1.5e+7 1.0e+7 5.0e+6 BkF R 2 = e+6 6.0e+6 5.0e+6 4.0e+6 3.0e+6 2.0e+6 1.0e+6 BeF R 2 = The Mass Injected to the GC/MS(ng) Integrated Area 2.5e+7 2.0e+7 1.5e+7 1.0e+7 5.0e+6 BaP R 2 = e+6 6.0e+6 5.0e+6 4.0e+6 3.0e+6 2.0e+6 1.0e+6 PER R 2 = The Mass Injected to the GC/MS(ng) BkF, BeP, BaP PER -99-

115 Integrated Area 2.0e+7 1.5e+7 1.0e+7 5.0e+6 IND R 2 = e+6 5.0e+6 4.0e+6 3.0e+6 2.0e+6 1.0e+6 DBA R 2 = The Mass Injected to the GC/MS(ng) Integrated Area 1.6e+6 1.2e+6 8.0e+5 4.0e+5 BbC R 2 = e+7 8.0e+6 4.0e+6 BghiP R 2 = The Mass Injected to the GC/MS(ng) IND, DBA, BbC BghiP -100-

116 Integrated Area 6.0e+6 4.0e+6 2.0e+6 COR R 2 = The Mass Injected to the GC/MS(ng) COR -101-

117 4-4-1 PAHs (Chem Service) (µg ml -1 ) Acenaphthene Acp 2000 Fluoranthene FL 2000 Naphthalene Nap 2000 Benzo(a)anthracene BaA 2000 Benzo(a)pyrene BaP 2000 Benzo(b)fluoranthene BbF 2000 Benzo(k)fluoranthene BkF 2000 Chrysene (93%) CHR 2000 Acenaphthylene AcPy 2000 Anthracene Ant 2000 Benzo(ghi)perylene BghiP 2000 Fluorene Flu 2000 Phenanthrene PA 2000 Dibenzo(a,h)anthracene DBA 2000 Indeno(1,2,3-cd)pyrene IND 2000 Pyrene Pyr 2000 Perylene PER 100 Benzo(e)pyrene BeP 100 Coronene COR PAHs (Gravimetric Certificate) (µg ml -1 ) Cyclopenta(c,d)pyrene CYC 10 Benzo(b)chrysene BbC

118 PAHs PAHs 10 µg ml -1 GC/MS Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR

119 4-4-4 PAHs 10 µg ml -1 GC/MS PAHs (%) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR

120 S X i Xn n ± 4.55% ~ ± 3.93% 0.27% ~ 9.15% ( 4-5-2) 4-6 PAHs 3 3 (SD) ± 3 SD GC/MS SCAN mode (Primary ion number) (Secondary ion number) SIM mode (Selectivity ion monitoring mode) 21 PAHs GC/MS (SD) 3 SD 21 PAHs GC/MS GC/MS SIM mode SIM mode (Primary ion) (Secondary ion)

121 PAHs (%) (%) (%) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR

122 4-5-2 PAHs PAHs (%) (%) (%) (%) Nap ± 13.9 AcPy ± 4.55 Acp ± 8.63 Flu ± 14.7 PA ± 6.35 Ant ± 7.35 FL ± 6.50 Pyr ± 8.19 CYC ± 9.74 BaA ± 5.18 CHR ± 13.2 BbF ± 13.8 BkF ± 4.45 BeP ± 1.99 BaP ± 1.27 PER ± 11.3 IND ± 10.1 DBA ± 3.93 BbC ± 11.6 BghiP ± 0.53 COR ±

123 PAHs GC/MS (min) PAHs Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR

124 PAHs GC/MS PAHs 3SD (min) (SD) (min) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR

125 PAHs (Primary ion) (Secondary ion) PAHs Primary ion Secondary ion Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR

126 4-7 ( ) -111-

127 ~10 ( ) 10 11~12 ( ) 12 24~25 ( ) ~12 ( ) PAHs A C D E F G C E G E F G A B C D (µg m -3 ) A B C D E F G A 38.6~142 µg m µg m -3 B 112 µg m -3 C 37.2~141 µg m µg m -3 D 21.1~129 µg m µg m -3 E 39.3~191 µg m µg m -3 F 48.4~120 µg m µg m -3 G 45.7~90.5 µg m µg m (250 µg m -3 ) (1994) (112, 122 µg m -3 ) (2000) -112-

128 (148, 237, µg m -3 ) Concentration (µg m -3 ) Spring Summer Fall Winter 50 0 A B C D E F G Sampling sites µg m

129 (Mixing height) (Boundary layer) 2000 (1992) PAHs PAHs ~ PAHs ( + ) F (666 ng m -3 ) D (235 ng m -3 ) PAHs (1993) 1794 ng m -3 (1998) 1496 ng m -3 (1995) 1324 ng m -3 (1998) ( ng m -3 ) (1996) ( ng m -3 ) (1998) ( ng m -3 ) PAHs PAHs -114-

130 PAHs (ng m -3 ) PAHs Site A (n=2) Site B (n=1) Site C (n=3) Site D (n=2) Site E (n=3) Site F (n=2) Site G (n=3) Nap 332 (223~441) (70~680) 203 (24~382) 456 (15~836) 618 (49~1187) 398 (15~756) AcPy 4.03 (3.30~4.75) (1.46~3.19) 1.52 (0.60~2.43) 4.51 (0.12~12.7) 6.32 (1.79~10.8) 3.78 (0.10~10.0) Acp 5.3 (5.25~5.34) (8.23~10.1) 2.37 (0.72~4.0) 3.23 (0.29~6.57) 3.21 (0.10~6.31) 2.38 (0.28~4.83) Flu 10 (9.53~10.5) (12.2~13.8) 5.68 (3.18~8.17) 8.33 (0.96~17.1) 4.71 (3.32~6.09) 6.86 (0.48~14.7) PA 23 (20.7~25.2) (22.5~31.0) 10.9 (5.05~16.6) 15.8 (2.86~30.9) 16.8 (11.3~22.3) 14.6 (4.72~28.3) Ant 1.89 (1.07~2.71) (1.52~2.29) 0.89 (0.73~1.05) 0.41 (0.29~0.61) 0.72 (0.26~1.17) 0.58 (0.29~0.70) FL 6.08 (5.61~6.53) (5.51~8.33) 2.87 (1.31~4.43) 3.09 (0.55~5.21) 4.82 (0.92~8.72) 3.14 (0.69~6.25) Pyr 3.21 (0.73~5.68) (3.86~6.10) 2.06 (0.40~3.70) 2.97 (0.44~5.64) 5.71 (5.44~5.97) 2.98 (0.50~6.34) CYC 0.1 (0.16~0.02) (0.006~0.22) 0.09 (0.16~0.20) 0.15 (0.03~0.28) 0.04 (0.02~0.06) 0.37 (0.19~0.56) BaA 0.25 (0.11~0.39) (0.05~0.35) 0.13 (0.059~0.20) 0.07 (0.003~0.10) 0.03 (0.01~0.05) 0.69 (0.08~1.05) CHR 0.73 (0.17~1.29) (0.33~1.26) 0.98 (0.28~1.676) 0.63 (0.003~0.99) 0.36 (0.003~0.72) 1.39 (0.30~2.91) BbF 0.1 (0.04~0.14) (0.02~0.29) 0.2 (0.09~0.29) 0.59 (0.46~0.74) 0.24 (0.07~0.41) 1.51 (1.05~2.05) BkF 0.16 (0.14~0.16) (0.21~0.41) 0.23 (0.18~0.27) 0.68 (0.13~1.08) 0.44 (0.06~0.81) 1.63 (1.22~2.37) BeP 0.24 (0.16~0.31) (0.16~0.83) 0.88 (0.66~1.10) 1 (0.56~1.42) 0.63 (0.16~1.09) 1.56 (0.61~2.21) BaP 0.12 (0.06~0.18) (0.091~0.31) 0.08 (0.026~0.14) 0.5 (0.19~0.77) 0.78 (0.017~1.54) 0.85 (0.22~1.62) PER 0.13 (0.073~0.19) (0.13~0.42) 0.8 (0.67~0.92) 0.49 (0.09~1.12) 0.35 (0.016~0.69) 0.33 (0.04~0.53) IND 0.2 (0.053~0.35) (0.04~0.17) 0.44 (0.06~0.82) 0.79 (0.70~0.86) 0.33 (0.30~0.34) 1.35 (1.05~1.83) DBA 0.02 (0.008~0.03) (0.07~0.52) 0.15 (0.12~0.16) 0.3 (0.04~0.58) 0.3 (0.04~0.54) 0.34 (0.08~0.55) BbC 0.2 (0.13~0.27) (0.06~0.29) 0.17 (0.15~0.19) 0.41 (0.08~0.89) 0.88 (0.02~1.74) 0.21 (0.15~0.25) BghiP 0.08 (0.005~0.15) (0.006~0.48) 0.38 (0.20~0.55) 0.52 (0.17~0.91) 0.08 (0.004~0.15) 1.29 (0.30~2.22) COR 0.78 (0.45~1.10) (0.36~1.04) 0.77 (0.50~1.04) 1.13 (0.64~1.40) 0.98 (0.05~1.90) 1.74 (1.39~1.92) Total

131 5-1-3 PAHs (ng m -3 ) PAHs + 1 N.A. N.A. 508 (1998) 2 N.A. N.A. 442 (1998) (1993) (1996) (1996) (1998) (1994) (1994) N.A. N.A. 198 (1998) N.A. N.A. 298 (1998) (1995) (1995) N.A PAHs PAHs PAHs PAHs PAHs PAHs PAHs A~G ( / + ) 1.76% 2.15% 1.77% 3.97% 2.84% 1.09% 4.14% PAHs (7.35~16.7%) PAHs PAHs PAHs -116-

132 (Blow-off) PAHs PAHs PAHs Bidleman, 1986 (1998) PAHs 1274 ng m -3 PAHs 222 ng m -3 PAHs 85% PAHs 15% PAHs PAHs (Nap AcPy Acp Flu PA) (1998) PAHs 4 (MW 252) PAHs Grojean, 1983 PAHs PAHs PAHs ; PAHs Vaeck et al.,

133 PAHs (Cp) (Cg) PAHs A (n=2) B (n=1) C (n=3) D (n=2) Cg Cp Cp / Cg Cp Cp / Cg Cp Cp / Cg Cp (ng m -3 ) (ng m -3 ) PAHs (%) (ng m -3 ) (ng m -3 ) PAHs (%) (ng m -3 ) (ng m -3 ) PAHs (%) (ng m -3 ) (ng m -3 ) Cp / PAHs (%) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR Total

134 PAHs (Cp) (Cg) PAHs ( ) E (n=3) F (n=2) G (n=3) Cg Cp Cp / Cg Cp Cp / Cg Cp (ng m -3 ) (ng m -3 ) PAHs (%) (ng m -3 ) (ng m -3 ) PAHs (%) (ng m -3 ) (ng m -3 ) Cp / PAHs (%) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR Total

135 PAHs PAHs 21 PAHs Nap 2 3 PAHs Acpy Acp Flu PA Ant 4 PAHs FL Pyr BaA CHR 5 PAHs CYC BbF BkF BeP BaP PER DBA BbC 6 PAHs IND Bghip 7 PAHs COR PAHs ( Nap) 3 PAHs C (75.7 ng m -3 ) A (75.6 ng m -3 ) ( 687 ng m -3 ) ( 115 ng m -3 ) PAHs (Aceves, ) Müller (1998) PAHs 3~6 PAHs Dörr (1996) PAHs 1.9~14 Müller (1998) Dörr (1996) PAHs ( Nap) 3 PAHs 79% 4 PAHs 5~7 PAHs

136 rings A B C D E F G rings A B C D E F G 20 5 PAHs concentration (ng m -3 ) 0 0 spring summer fall winter A 10 5-rings 6-rings spring summer fall winter spring summer fall winter B C D E F G spring summer fall winter A B C D E F G rings A A B B C C D D E E F F G G Total PAHs A B C D E F G spring summer fall winter 0 spring summer fall winter Season Season PAHs -121-

137 A 119~215 mg m -2 day mg m -2 day -1 B 148~205 mg m -2 day mg m -2 day -1 C 91~183 mg m -2 day mg m -2 day -1 D 121~209 mg m -2 day mg m -2 day -1 E 102~207 mg m -2 day mg m -2 day -1 F 70~181 mg m -2 day mg m -2 day -1 G 69~259 mg m -2 day mg m -2 day Holsen et al., 1991; Lee, 1991; Fang, 1992; Lin et al., (2000) -122-

138 (a) Dry depostion flux (mg m -2 day -1 ) Spring Summer Fall Winter 0 A B C D E F G Sites (b) Dry depostion velocity (cm s -1 ) Spring Summer Fall Winter 0 A B C D E F G Sites (a) (b) -123-

139 5-2-1 (mg m -2 day -1 ) 142~ Noll et al., ~ Lee, ~ Holsen and Noll, ~ Lin et al., ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ V d,tm =K (F T,TM ) (C TSP ) (5-1) V d,tm = (cm s -1 ) K = F T,TM = (mg m -2 day -1 ) C TSP = (µg m -3 ) -124-

140 5-2-1 (b) A 1.68~6.44 cm s cm s -1 B 1.53 cm s -1 C 1.50~2.91 cm s cm s -1 D 1.87~9.81 cm s cm s -1 E 0.61~6.10 cm s cm s -1 F 0.81~3.33 cm s cm s -1 G 0.89~2.38 cm s cm s Fang (1996) (cm s -1 ) Tunghai University 6.93 Jongieng Elementary School 9.21 Fang, 1996 Shingang Elementary School

141 5-2-2 PAHs PAHs PAHs PAHs PAHs PAHs A PAHs 88.0~190 µg m -2 day µg m -2 day -1 B 108~202 µg m -2 day µg m -2 day -1 C 63.4~260 µg m -2 day µg m -2 day -1 D 94.9~181 µg m -2 day µg m -2 day -1 E 99.7~419 µg m -2 day µg m -2 day -1 F 88.0~355 µg m -2 day µg m -2 day -1 G 83.7~210 µg m -2 day µg m -2 day -1 (1996) PAHs (131~194 µg m -2 day -1 ) 400 Dry deposition flux (µg m -2 day -1 ) A B C D E F G Sampling sites PAHs -126-

142 5-3 ( ) PAHs 1999 McVeety Hites (1988) PAHs 9 1 PAHs ~ A~G PAHs PAHs Nap 331~909 ng L -1 Nap 20 PAHs ( µg L -1 ) Nap PAHs PAHs ng L ~619 ng L -1 PAHs 202~3296 ng L ~1267 ng L -1 (1999) PAHs ( ng L ng L -1 ) PAHs PAHs PAHs PAHs PAHs ( 24 ) ( 30 ) -127-

143 PAHs PAHs (ng L -1 ) A (n=4) B (n=4) C (n=4) D (n=4) E (n=4) F (n=4) G (n=4) Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR Total

144 5-3-2 PAHs A B C D E F G PAHs 416~ ~ ~ ~ ~ ~ ~868 ng L PAHs (%) 222~ ~ ~ ~ ~ ~ ~1494 ng L PAHs (%) 3500 Wet deposition conc. (ng L -1 ) R 2 = n = Concentration (ng m -3 ) PAHs PAHs -129-

145 PAHs PAHs PAHs PAHs (57.2~70.8%) PAHs (67.8~71.3%) Franz (1998) PAHs PAHs 2~4 PAHs PAHs PAHs PAHs 5-4 D D G PAHs D G 2.5 µm (Coarse particles) (Fine particles) (Respirable particles PM 2.5 ) 2.5 µm (Coarse mode) (Accumulation mode) (Nucleation mode) Watson, 1998a; Lundgren and Burton, D 0.31~0.52 µm 3.2~5.6 µm -130-

146 µg m -3 D 0.31~0.52 µm 1~1.8 µm 3.2~5.6 µm µg m -3 G 0.166~0.31 µm 0.52~1 µm 3.2~5.6 µm µg m ~ ~3.2 µm (Acumulative mode) Vaeck et al., 1979; Aceves et al., PAHs PAHs D 0.31~0.52 µm 5.6~10 µm G 0.166~0.31 µm 10~18 µm PAHs PAHs PAHs PAHs PAHs 10 µm PAHs 1.0~3.2 µm 2.5 PAHs -131-

147 Total particle mass D-summer D-winter dc/dlogdp (µg m -3 ) G-winter Particle diameter (µm)

148 60 Total PAHs dc/dlogdp (ng m -3 ) D-summer Particle diameter (µm) dc/dlogdp (ng m -3 ) G-winter Particle diameter (µm) PAHs -133-

149 5-4-3 PAHs (%) MMD (Mass median diameter 50% ) (Geometric standard deviation) PAHs D 1.0 µm 3.2 µm 10 µm 33.0% 55.1% 76.6% D 1.0 µm 3.2 µm 10 µm 45.0% 68.2% 88.9% G 1.0 µm 3.2 µm 10 µm 46.9% 71.8% 89.9% PAHs D 1.0 µm 3.2 µm 51.2% 71.0% D 1.0 µm 3.2 µm 45.1% 68.8% G 1.0 µm 3.2 µm 48.7 % 69.1% 2.5 µm PAHs 2.5 µm Venkataraman (1994) Vaeck (1979) Katz Chan (1980) Vaeck Cauwenberghe (1985) (1996) PAHs ( 2.5 µm ) PAHs 69.8% 65.0% PAHs 60% 1.0 µm PAHs 48.4% 3 (Submicron) g -134-

150 Total particle mass Cumulation fraction (%) D-summer D-winter G-winter Particle diameter (µm) Total PAHs Cumulation fraction (%) D-summer D-winter G-winter Particle diameter (µm) PAHs -135-

151 5-4-4 PAHs MMD g (Mass median diameter, MMD) ( PAHs) 50% ( d 50 ) MMD o MMD D D G PAHs MMD o µm D D G MMD o µm PAHs MMD o MMD o 21 PAHs MMD o MMD o PAHs PAHs 1.0 µm MMD o MMD o MMD f MMD c (Find-particle mode 0.166~1.8 µm ) (Coarse-particle mode 1.8~18 µm ) PAHs MMD f D D G µm MMD f D D G µm 21 PAHs MMD f 0.312~0.703 µm 0.301~1.02 µm 0.202~0.608 µm MMD f 0.20~1.1 µm PAHs MMD c D D G µm MMD c D D G µm 21 PAHs MMD c 3.96~10.1 µm 3.24~10.2 µm 4.18~10.1 µm MMD c 3.0~11.0 µm (Geometric standard deviation, g ) -136-

152 ( PAHs) g d d 84 g = = 50 d d 50 σ (5-2) 16 d 84 = ( PAHs) 84% d 50 = ( PAHs) 50% d 16 = ( PAHs) 16% g,c g,f D D G PAHs 21 PAHs g,c 1.30~ ~ ~2.66 g,f 1.30~ ~ ~2.69 PAHs PAHs 21 PAH g,o D D G 1.15~ ~ ~

153 5-4-1 PAHs MMD o (µm) Site D- Summer D- Winter G- Winter PAHs MMD o g,o MMD o g,o MMD o g,o Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR PAHs g,o -138-

154 5-4-2 PAHs MMD (µm) Sites D- Summer D- Winter G- Winter PAHs MMD c σ g,c MMD f σ g,f MMD c σ g,c MMD f σ g,f MMD c σ g,c MMD f σ g,f Nap AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR PAHs g

155 5-5 PAHs ISCST3 PAHs 20 PAHs CMB CMB ISCST3 ISCST3 PAHs Trinity Breeze Air ISCST3 (Version 1.12) ISC ISCST ISCST3 ISCST3 UTM (m) (g s -1 ) (m) (K) (m s -1 ) (m) PAHs

156

157 5-5-2 ISC -142-

158 5-5-1 (m) (g s -1 ) (m) (K) (m s -1 ) (m) x y z PAHs ISCST3 UTM (m) x y z A B C D E F G km 10 km 1 1 ISCST3 (K) (m s -1 ) -143-

159 (1992) ISCST3 ISCST3 (µg m -3 ) ISCST ISCST3 PAHs A~G ~ 0.330% PAHs -144-

160 5-5-3 ISCST3 PAHs M/R (R) (M) µg m -3 µg m -3 µg m -3 % Deg (90/7/3~7/4) A (90/11/11~10/12) (90/12/24~12/25) (91/03/11~03/12) (90/7/3~7/4) B (90/11/11~10/12) (90/12/24~12/25) (91/03/11~03/12) (90/7/3~7/4) C (90/11/11~10/12) (90/12/24~12/25) (91/03/11~03/12) (90/7/3~7/4) D (90/11/11~10/12) (90/12/24~12/25) (91/03/11~03/12)

161 5-5-3 ISCST3 PAHs ( ) M/R (R) (M) µg m -3 µg m -3 µg m -3 % Deg E (90/7/3~7/4) (90/11/11~10/12) (90/12/24~12/25) (91/03/11~03/12) (90/7/3~7/4) F (90/11/11~10/12) (90/12/24~12/25) (91/03/11~03/12) (90/7/3~7/4) G (90/11/11~10/12) (90/12/24~12/25) (91/03/11~03/12)

162 5-5-2 PAHs (Profile) PAHs PAHs PAHs (Profile) PAHs Dörr et al., 1996; Daisey et al., 1986 PAHs PAHs Daisey et al., 1986; Khalili et al., 1995; Dörr et al., 1996 Dörr (1996) PAHs CMB (Augsburg) PAHs PAHs Müller (1998) (Brisbane) PAHs PAHs PAHs PAHs (Bap/Bghip) PAHs PAHs Quraishi, 1985 PAHs PAHs Cretney et al., 1985; Cheng and Richard,

163 (Pb) PAHs Pb Daisey (1986) BeP PAHs BeP PAHs PAHs PAHs PAHs PAHs ( ) PAHs PAHs ( ) PAHs PAHs PAHs PAHs 20 PAHs ( Nap) PAHs PAHs 3 PAHs (Acpy, Acp, Flu, PA, Ant) PAHs 21 PAHs 20 PAHs ( Nap) (Cluster analysis) (Chi-square test) -148-

164 5-5-4 PAHs BghiP/COR Pyr/BaP Pyr/BeP BaA/BaP BaP/BghiP COR/BeP Bghip/BeP BaP/BeP CHR/BeP BkF/IND IND/BghiP 1.5 2~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~1.8 1~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ Bjørseth and Ramdahl, 1985; Daisey et al., 1986; Masclet et al., 1986; Pyysalo et al., 1987; Yang et al., 1991; Beak et al., 1991; Aceves and Grimalt, 1993; Li and Kamens, 1993, Smith and Harrison, 1996; Nielsen et al., 1996; Pandey et al., 1999; Caricchia et al., 1999; Panther et al., 1999; Kim Oanh et al., 2000; Park et al.,

165 5-5-5 PAHs A1 A4 B4 C1 C2 C3 D1 D4 E1 E2 E3 F1 F3 G1 G2 G3 BghiP/COR Pyr/BaP Pyr/BeP BaA/BaP BaP/BghiP COR/BeP Bghip/BeP BaP/BeP CHR/BeP BkF/IND IND/BghiP

166 A-summer A-spring C-summer C-spring C-fall PAHs/Total PAHs (%) D-summer D-spring E-summer E-winter F-summer F-winter AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR G-summer G-fall G-winter PAHs B-spring PAHs

167 PAHs SAS (Statistical analysis system) 8.0 (Ward s minimum variance method) ( ) ( ) (Fusion) A B C D E F G PAHs -152-

168 (Categorical data) ( ) ( ) (Two factor contingency table) ( -153-

169 ) 16 PAHs ( Nap 20 PAHs PAHs ) PAHs 95% PAHs PAHs G ( ) F ( ) G F G F PAHs A1 A2 B1 C1 C2 C3 D1 D2 E2 E3 E4 F2 F4 G2 G3 G

170 5-5-3 CMB PAHs ( ) PAHs PAHs (1) % 0.5% 6 PAHs (1998) PAHs ( 30 ton hr -1 ) ( 10 ~ 30 ton hr -1 ) ( 10 ton hr -1 ) PAHs mg L -1 ( 3-10 ) (1999) PAHs PAHs 6.13 mg L -1 ( 3-10 ) PAHs (1999) (1998) PAHs -155-

171 ( ) PAHs ( ) (2) Li et al. (1999) PAHs 3.43 mg ton mg m -3 ( ) Li et al. (1999) PAHs ( ) (3) 800~1000 (1999) PAHs 4350 mg ton -1 ( ) PAHs ( ) (4) Li et al. (1999) PAHs 2920 mg ton mg m -3 ( ) (5) PAHs -156-

172 900 tons m de-nox PAHs 125 µg m -3 ( ) -157-

173 µg L -1 (ton hr -1 ) mg m -3 mg ton -1 mg ton -1 mg ton -1 mg m -3 µg m -3 µg L ~30 10 Nap AcPy Acp Flu Ant PA FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND ND ND DBA BbC BghiP ND ND COR ND Total PAHs Li et al. Li, et al. (1999) (1998) (1999) (1999) (1999) ND -158-

174 PAHs PAHs (1998) ( ) PAHs PAHs (1) (1998) PAHs ECE-R PAHs mg kl -1 (2) (1998) (1000 rpm) 40 km hr -1 (1500 rpm) 80 km hr -1 (2200 rpm) 120 km hr -1 (3000 rpm) 25 Mazda-E (OHC) Borghi & Saveri FE-150S PC 150 HP (Super-2170) (API=SH, 10W/40) -159-

175 (95-lead free gasoline, 95-LFG) PAHs 5680 mg kl (3) (1998) Honda 125 c.c. Honda 50 c.c (92-lead free gasoline, 92-LFG) PAHs mg kl -1 PAHs mg kl

176 PAHs (mg kl -1 ) Nap AcPy Acp Flu Ant PA FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR Total PAHs

177 (Speed) (Mode) (rpm) (Load) (%) (Weighting Factor) (%) 1 Idle (rpm) (A) (kg-m) (kw) (hp) (PS) (%) N.A. N.A. N.A N.A. N.A. N.A. N.A (Honda 50 c.c.) 5000 km 92-LFG (Honda 125 c.c.) km 92-LFG km hr -1 (6500 rpm) (2% 5%) (Idling) 60 km hr -1 (8000 rpm) (Idling) 40 km hr -1 (2500 rpm) 60 km hr -1 (4000 rpm) -162-

178 PAHs 1. PAHs ( PAHs ) USEPA USEPA, PAHs -163-

179 ( ) ( ) PAHs PAHs Q = F E (5-3) Q = PAHs F = E = PAHs PAHs PAHs ( ) PAHs -164-

180 5-5-5 PAHs -165-

181 5-5-6 PAHs -166-

182 PAHs PAHs PAHs PAHs PAHs Nap PAHs AcPy Acp Flu Ant PA PAHs FL Pyr BaA CHR PAHs CYC BbF BkF BeP BaP PER DBA BbC PAHs IND Bghip PAHs COR PAHs PAHs (LMW) PAHs PAHs (MMW) PAHs PAHs (HMW) PAHs PAHs PAHs (56.7%) (24.7%) PAHs ,895 ( 45.8%) 247,058 ( 22.4%) 281,801 ( 25.5 %) 12,346 ( 1.11%) 1,103,640 ( 3-27) ( ) -167-

183 PAHs kg yr -1 LMW MMW HMW Total PAHs % PAHs , , , ,058 (km L ) (km week ) (km week ,200 43,474 ) 7,716 2,749 2,443 ( ) 192,927 4, ,105 64,991 26,

184 , ,921 10,901 2% 716,589 kl 30.0% 57.0% 9.07% 3.66% ( ) ( ) ( ) ,537 17,550 62, ,515 17,781 56, ,375 19,663 63, ,049 16,260 57, ,657 18,619 63, ,096 18,384 60, ,134 19,002 63, ,755 18,161 62, ,833 15,784 56, ,937 18,265 61, ,729 18,006 58, ,304 18,593 61, , , ,

185 ( ) 216, ,797 64,991 26, , PAHs PAHs PAHs 8,037 2, , PAHs PAHs Nap PAHs AcPy Acp Flu Ant PA PAHs FL Pyr BaA CHR PAHs CYC BbF BkF BeP BaP PER DBA BbC PAHs IND Bghip PAHs COR PAHs PAHs (LMW) PAHs PAHs (MMW) PAHs PAHs (HMW) PAHs 7,784 1, , PAHs 64.3 % 18.6% 6.83% 10.3% PAHs 75% -170-

186 PAHs PAHs (kg yr -1 ) Nap 6, ,209 AcPy Acp Flu Ant PA FL Pyr BaA CHR CYC BbF BkF BeP BaP PER DBA BbC IND BghiP COR Total PAHs 8,037 2, ,

187 PAHs (kg yr -1 ) PAHs 6, ,209 1,086 1, LMW 7,784 1, ,274 MMW HMW PAHs (%) PAHs PAHs

188 PAHs PAHs PAHs PAHs (n=16) PAHs PAHs PAHs PAHs PAHs Average Inventory Emission (kg day -1 ) Inventory Emission Measured PAHs concentration Average concentration (ng m -3 ) AcPy Acp Flu PA Ant FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR PAHs PAHs PAHs -173-

189 5-5-4 (CMB) CMB CMB (Source profile) (Fingerprint) CMB 8.0 PAHs PAHs PAHs CMB 8.0 CMB 8.0 PAHs PAHs CMB 8.0 PAHs PAHs CMB 8.0 CMB CMB PAHs PAHs PAHs ( ) PAHs CMB 8.0 PAHs PAHs 20 PAHs ( Nap) PAHs F ij = [PAH i ] / [PAH total ] PAHs (%) PAHs DBA IND 19.6% 15.4% Ant FL -174-

190 59.1% 12.2% Ant AcPy 35.3% 18.7% FL Pyr 67.5% 6.51% Ant Pyr 35.9% 8.67% Flu AcPy 27.1% 17.5% PAHs CMB PAHs PAHs 95% PAHs CMB

191 PAHs (%) PAHs AcPy Acp Flu Ant PA FL Pyr CYC BaA CHR BbF BkF BeP BaP PER IND DBA BbC BghiP COR Total Li et al. (1998) (1999) (1999) (1999) (1998) -176-

192 PAHs CMB 8.0 CMB CMB 8.0 CMB 8.0 ( ) 20 ( + ) PAHs 20 PAHs ( + ) CMB PAHs CMB 8.0 (16 ) (93.4 %) R R ~339 ng m ~135% ( 5-5-8) 22.5% (N.A.~50.2%) 1.27 % (N.A.~7.3%) 25.4% (N.A.~100%) 9.67% (N.A.~86.5%) 1.21% (N.A.~18.2%) 40.0% (N.A.~82.4%) 80~120% ( ) E G ( ) G 38~60% PAHs CMB

193 (ng m -3 ) CMB PAHs (ng m -3 ) R 2 (%) A 2001/07/ A 2002/03/ N.A. N.A. N.A. N.A B 2002/03/ N.A. N.A. N.A. N.A C 2001/07/ N.A. N.A. N.A. N.A C 2001/10/ N.A N.A. N.A. N.A. 120 C 2002/03/ N.A N.A. N.A D 2001/07/ N.A. N.A. N.A. N.A D 2002/03/ N.A E 2001/07/ N.A N.A. N.A E 2001/10/ N.A. N.A E 2001/12/ N.A N.A. N.A. 112 F 2001/07/ N.A. N.A. N.A. N.A F 2001/12/ N.A N.A. N.A G 2001/07/ N.A. N.A N.A. N.A. N.A G 2001/10/ N.A N.A. N.A G 2001/12/ N.A (1)N.A. (2) T-Statistic

194 Contribution percentage (%) Mobile Oil Gas Coal Deisel MSWI 1 : 2001/07/09 2 : 2001/10/11 3 : 2001/12/24 4 : 2002/03/11 0 A1 A4 B4 C1 C2 C4 D1 D4 E1 E2 E3 F1 F3 G1 G2 G3 Sampling sites PAHs 8 PAHs PAHs PAHs Mastclet et al., 1986 Pitts et al. (1978) PAHs CMB CMB CMB PAHs Kamens et al., 1985, 1988 PAHs PAH PAHs (FL Pyr BaA CHR BbF BkF BeP -179-

195 COR) PAHs CMB 8.0 PAHs 20 PAHs 8 PAHs CMB PAHs (62.5%) R R N.A.~21.6 ng m -3 N.A.~140% ( 5-5-9) 17.6% (N.A.~92.%) 20.3% (N.A.~100%) 24.4% (N.A.~89.1%) 0.43% (N.A.~4.23%) 12.3% (N.A.~86.7%) 18.9% (N.A.~95.6%) 20 PAHs 8 PAHs R 2 PAHs % 80~120% PAHs 20 PAHs CMB 20 PAHs PAHs ( + ) PAHs -180-

196 (ng m -3 ) CMB PAHs (ng m -3 ) R 2 (%) A 2001/07/ N.A A 2002/03/ N.A. N.A N.A B 2002/03/ N.A. N.A. N.A. 113 C 2001/07/ N.A N.A C 2001/10/ N.A N.A. N.A C 2002/03/ N.A. N.A. N.A. 140 D 2001/07/ N.A. N.A. N.A. N.A D 2002/03/ N.A N.A. N.A. N.A. 101 E 2001/07/ N.A. N.A. N.A N.A E 2001/10/ N.A N.A. N.A E 2001/12/ N.A N.A. N.A F 2001/07/ N.A. N.A. 119 F 2001/12/ N.A N.A. N.A. N.A. N.A G 2001/07/ N.A. N.A. N.A. N.A. N.A. N.A. 0 G 2001/10/ N.A N.A. N.A. N.A G 2001/12/ N.A. N.A N.A (1)N.A. (2) T-Statistic

197 Contribution percentage (%) Mobile Oil Gas Coal Deisel MSWI 1 : 2001/07/09 2 : 2001/10/11 3 : 2001/12/24 4 : 2002/03/11 0 A1 A4 B4 C1 C2 C4 D1 D4 E1 E2 E3 F1 F3 G1 G2 G3 Sampling sites PAHs CMB PAHs (25%) R ~34.5 ng m ~176% 79.5% (25.5~100%) 0.28% (N.A.~4.46%) 5.23% (N.A.~34.1%) N.A % (N.A.~7.84%) 14.4 % (N.A.~61.9%) 20 PAHs 8 PAHs 20 PAHs R 2 ( 0.437) PAHs PAHs -182-

198 PAHs 8 PAHs PAHs 8 PAHs CMB PAHs R R 2 20 PAHs 8 PAHs CMB -183-

199 (ng m -3 ) CMB PAHs (ng m -3 ) R 2 (%) A 2001/07/ N.A N.A. N.A A 2002/03/ N.A. N.A. N.A. N.A. N.A. 112 B 2002/03/ N.A. N.A. N.A. N.A C 2001/07/ N.A. N.A. N.A. N.A C 2001/10/ N.A N.A C 2002/03/ N.A N.A. N.A D 2001/07/ N.A N.A. N.A D 2002/03/ N.A. N.A. N.A. N.A. N.A E 2001/07/ N.A. N.A. N.A. N.A E 2001/10/ N.A. N.A. N.A. N.A. N.A. 133 E 2001/12/ N.A. N.A. N.A. N.A F 2001/07/ N.A F 2001/12/ N.A. N.A. N.A. N.A. N.A G 2001/07/ N.A N.A. N.A G 2001/10/ N.A. N.A. N.A. N.A. N.A. 128 G 2001/12/ N.A. N.A. N.A. N.A. N.A. 158 (1)N.A. (2) T-Statistic

200 CMB PAHs (ng m -3 ) (ng m -3 ) R 2 (%) A 2001/07/ N.A. N.A N.A. N.A A 2002/03/ N.A N.A. N.A B 2002/03/ N.A. N.A N.A. N.A C 2001/07/ N.A. N.A N.A C 2001/10/ N.A. N.A N.A. N.A C 2002/03/ N.A. N.A N.A. N.A D 2001/07/ N.A. N.A N.A D 2002/03/ N.A N.A. N.A E 2001/07/ N.A. N.A N.A. N.A E 2001/10/ N.A. N.A N.A. N.A E 2001/12/ N.A N.A. N.A. N.A. 139 F 2001/07/ N.A. N.A N.A F 2001/12/ N.A N.A G 2001/07/ N.A G 2001/10/ N.A. N.A N.A N.A G 2001/12/ N.A. N.A N.A. N.A. N.A (1)N.A. (2) T-Statistic

201 ISCST3 CMB 8.0 ISCST3 PAHs CMB PAHs PAHs 40% (n =16 N.A.~82.4% ) CMB PAHs ( + ) (93.4%) R R ~355 ng m ~125% ( ) 36.5% (N.A.~49.0%) 4.03% (N.A.~16.9%) 47.9% (13.6~100%) 8.33% (N.A.~73.4%) 3.21% (N.A.~21.8%) CMB 20 PAHs ( ) 22.4% 36.5% 1.26% 4.03% 25.3% 47.9% 9.67% 8.33% 1.20% -186-

202 3.21% 1.34% 2.01~22.6% ISCST3 CMB PAHs CMB

203 CMB PAHs - (ng m -3 ) (ng m -3 ) R 2 (%) A 2001/07/ A 2002/03/ N.A N.A B 2002/03/ N.A C 2001/07/ N.A C 2001/10/ N.A C 2002/03/ N.A D 2001/07/ N.A N.A D 2002/03/ N.A E 2001/07/ N.A N.A. N.A E 2001/10/ N.A E 2001/12/ N.A. 119 F 2001/07/ N.A F 2001/12/ N.A. 102 G 2001/07/ N.A. N.A N.A. N.A G 2001/10/ N.A. N.A G 2001/12/ N.A (1)N.A. (2) T-Statistic

204 Contribution percentage (%) Mobile Oil Gas Coal Deisel 1 : 2001/07/09 2 : 2001/10/11 3 : 2001/12/24 4 : 2002/03/11 0 A1 A4 B4 C1 C2 C4 D1 D4 E1 E2 E3 F1 F3 G1 G2 G3 Sampling sites PAHs ( MSWI) CMB CMB Peter and Richard (1993) Ground-based trajectories ( ) CMB Wadden et al., 1986; O Shea and Scheff, 1988; Peter and Richard, 1993 Peter and Richard (1993) Ground-based trajectories CMB (Graphic arts) VOCs (Gaussian plume model) -189-

205 C = 2 Q 1 y exp πuσ σ 2 σ y 1 z H exp 2 σ 2 y z z 2 (5-4) C = Q = u = z y = (z) (y) H = ( 10~70 km ) 10 km (Plume center line) y=0 z =Ax y =Gx x A G (5-1) 1.0 u ( m s -1 ) (5-5) α +γ C Q j / X (5-5) =1 ( ) -190-

206 Trajectory scores Q/X Q/X ± 22.5 Peter and Richard, 1993 Ground-based trajectores 70 km ( A~G) ± 22.5 ( ) (Q/X) CMB 8.0 PAHs ( ) Ground-based trajectores (0.855 kg km -1 day -1 ) ( kg km -1 day -1 ) ( kg km -1 day -1 ) (47.4 ) ( ) CMB 20 PAHs R CMB -191-

207 CMB CMB Trajectory score emission (Q/X) CMB CMB 8 PAHs CMB R PAHs CMB CMB CMB CMB CMB PAHs PAHs PAHs PAHs PAHs PAHs PAHs -192-

208

209 Spring Summer Fall Winter Mobile Oil Trajectory score, emission (kg km -1 day -1 ) e-3 A B C D E F G Gas A B C D E F G 0.0 A B C D E F G 0.3 Coal A B C D E F G 0.5 Diesel 0.4 MSWI 8.0e e A B C D E F G 0.0 A B C D E F G Sampling sites Sampling sites

210 MSWI 0.3 Oil R 2 = R 2 = Trajectory score, Emission (kg km -1 yr -1 ) R 2 = Mobile Gas Coal e-3 8e-4 6e-4 Deisel 0.1 4e-4 2e CMB coefficient (ng m -3 ) CMB coefficient (ng m -3 ) CMB 20 PAHs -195-

211 Trajectory score, Emission (kg km -1 yr -1 ) MSWI Mobile 2 R 2 = Coal Oil e-4 Gas e-3 8e-4 Deisel CMB coefficient (ng m -3 ) 4e-4 2e CMB coefficient (ng m -3 ) CMB 8 PAHs -196-

212 ~191 µg m µg m PAHs 235~666 ng m -3 PAHs ( / + ) 1.09~4.14% 2.53% PAHs PAHs (Nap AcPy Acp Flu PA) PAHs ~207 mg m -2 day mg m -2 day ~5.84 cm s cm s -1 PAHs 133 ~230 µg m -2 day µg m -2 day PAHs Nap 331~909 ng L -1 Nap 20 PAHs Nap 5. PAHs 105~1731 ng L -1 PAHs 202~3296 ng L -1 PAHs PAHs PAHs PAHs -197-

213 6. PAHs PAHs 2.5 µm 7. PAHs D D G 1.0 µm 3.2 µm 48.3% 69.8% 2.5 µm PAHs 69.8% 60% PAHs 1.0 µm PAHs 48.4% 3 PAHs 21 PAHs MMD MMD PAHs 8. ISCST3 PAHs PAHs PAHs 20 PAHs PAHs 9. CMB PAHs ( + ) 8 PAHs 20 PAHs 8 PAHs PAHs PAHs PAHs CMB PAHs -198-

214 10. CMB 8.0 CMB PAHs CMB PAHs PAHs PAHs PAHs 2. PAHs PAHs -199-

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235 -220- (1992) (1997) (1994) (1998) (1998) (1993) (1999) (1994) ABS (2001) (1992) (2000) (1998) (1995)

236 (1994) (1996) (1992) CMB 91 (2002) (1995) (1998) (1996) (1999) 3-34 (2000) (1992) (2000) (1999)

237 (1995) (1996) (1998) NSC B (1994) (1994) (1993) - E2 EPA-87-FA42-03.F5 (1998) (1999) (1999) (2000) (1996) -222-

238 (2000) PAHs (2001) -223-

239 -224-

240 CMB R-square / SCE µg/m 3 SCE STDERR (uncertainty) [ STDERR<<SCE] t- T-STAT STDERR SCE/STDERR[ 2] R 2 R-SQUARE 0 1 [ 0.8 1] X 2 CHI-SQUARE Chi-square [ 0 4] % Mass DF / (uncertainty/similarity U/S clusters) SUM (residual) R/U SCE [ 5] [ ] U/S clusters