title page

Contents

ABSTRACT 14

CHAPTER 1. Introduction 17

Motivation 17

Research Objectives 21

Approach 21

CHAPTER 2. Temporal trend and long range transport of particulate PAHs at Gosan 23

2.1. Introduction 23

2.2. Experimental 25

2.2.1. Sampling 25

2.2.2. Analysis 26

2.3. Results and Discussion 29

2.3.1. Temporal trend of particulate total PAHs concentrations 29

2.3.2. Comparison with other sites' results 31

2.3.3. Seasonal variation of the PAH compounds concentrations 36

2.3.4. Characteristics of air parcel movements 43

2.3.5. Relationship between the particulate PAHs and non-sea-salt (nss) SO₄²-(이미지참조) 52

2.4. Summary 55

CHAPTER 3. Temporal variation of particulate PAHs at Seoul 57

3.1. Introduction 57

3.2. Experimental 57

3.2.1. Sampling 57

3.2.2. Analysis 60

3.3. Results and Discussion 62

3.3.1. The level of particulate PAHs concentration at Seoul 62

3.3.2. Temporal variation of particulate PAHs concentrations at Seoul 66

3.3.3. Correlation between the particulate PAHs level with other air pollutants' concentrations 68

3.3.4. Correlation between particulate PAHs with ambient temperature 71

3.3.5. Source diagnostic ratios of PAHs 73

3.4. Summary 80

CHAPTER 4. Seasonal variation of particle size distributions of PAHs at Seoul, Korea 81

4.1. Introduction 81

4.2. Experimental 82

4.2.1. Sampling 83

4.2.2. Analysis 84

4.3. Results and Discussion 87

4.3.1. Size distribution of aerosol 87

4.3.2. Size distribution of PAHs 92

4.3.3. Source diagnostic ratios 99

4.4. Summary 102

CHAPTER 5. Dry deposition fluxes and overall deposition velocities of particulate PAHs 104

5.1. Introduction 104

5.2. Experimental 106

5.2.1. Sampling 106

5.2.2. Analysis 110

5.3. Results and Discussion 112

5.3.1. Dry deposition fluxes of particulate PAHs 112

5.3.2. Comparison of dry deposition fluxes of particulate PAHs with the previous result 118

5.3.3. Overall dry deposition velocities of PAHs 121

5.4. Summary 123

CHAPTER 6. Major sources to the particulate PAHs levels at Seoul, Korea 125

6.1. Introduction 125

6.2. CMB receptor model 126

6.3. Modeling 131

6.3.1. Measurement data 131

6.3.2. Source profile 133

6.4. Results and Discussion 146

6.4.1. The particulate PAHs levels at Seoul 146

6.4.2. General characteristics of the source apportionment result 147

6.4.3. Seasonal variation of the source apportionment results 151

6.5. Summary 158

CHAPTER 7. Overall conclusions 159

7.1. Summary and conclusions 159

7.2. Recommendations for future research 163

REFERENCES 165

ABSTRACT (KOREAN) 173

감사의 글 175

Table 1.1. Physical and chemical properties of 17 PAHs identified in this study (MOE, 2004). 19

Table 2.1. Particulate PAHs extraction recovery result and the NIST SRM-1649 urban… 29

Table 2.2. Comparison of particulate PAHs concentrations (pg m-³) in this study with the results measured at background and/or…(이미지참조) 34

Table 2.3. Seasonal difference of the concentrations (average ± standard deviation) of… 36

Table 2.4. Comparison of the BeP-to-BaP ratios in this study with other study results. 42

Table 2.5. Number of samples, the particulate PAHs concentration, and BeP/BaP ratio by air parcel trajectory. The values of… 47

Table 3.1. Particulate PAHs extraction recovery and analysis results of the NIST… 62

Table 3.2. Comparison of particulate PAHs concentrations (ng m-³) in this study with the results measured at urban areas…(이미지참조) 65

Table 3.3. Seasonal trend of the concentrations (average ± standard deviation) of… 68

Table 3.4. Source diagnostic ratios of particulate PAHs (Simcik et at., 1999). 74

Table 3.5. Comparison of the BeP-to-BaP ratios at Seoul with other study results. 79

Table 4.1. Summary of sampling and meteorological conditions in 2003. 83

Table 4.2. Size segregated particulate PAHs samples extraction recovery in this study and… 86

Table 4.3. The mass fraction of individual PAH compounds 92

Table 5.1. Summary of sampling and meterological conditions in 2003. 108

Table 5.2. The extraction recovery of dry deposition PAHs samples and analysis results of… 112

Table 5.3. Average dry deposition fluxes of particulate PAHs at Seoul 115

Table 5.4. Comparison of the measurement results for particulate PAHs dry deposition flux in Korea. 119

Table 5.5. Comparison of the measurement results for particulate PAHs dry deposition flux in the world. 120

Table 5.6. Comparison of the estimated dry deposition velocities for particulate PAHs 122

Table 6.1. Modeling performance measures(US EPA, 2004). 129

Table 6.2. Source composition of individual PAH compounds in particle phase. 145

Table 6.3. Modeling performance measures (Target values were set by US EPA, 2004). 149

Fig. 2.1. Map of this study site, Gosan, Jeju, Korea and other remote and urban sites in… 25

Fig. 2.2. Temporal trend of the particulate total PAHs concentrations and BeP-to-BaP… 31

Fig. 2.3. Comparison of the average concentrations of total particulate PAHs (sum of 7… 35

Fig. 2.4. Variation of the particulate total PAHs concentrations between 2001 and 2004 at… 44

Fig. 2.5. Variation of the average concentrations of individual PAH compounds by sector… 48

Fig. 2.6. Compositions of PAH compounds (individual PAH/ ∑ PAHs) (a) at Gosan by… 51

Fig. 2.7. Relationship between the concentrations of nss-SO₄²- concentrations and (a)…(이미지참조) 54

Fig. 3.1. Map of the sampling site at Seoul. 59

Fig. 3.2. Temporal variation of the particulate total PAHs concentrations between 2002 and 2003 at Seoul. 66

Fig. 3.3. The correlation of individual PAH compounds with air pollutants, (a) TSP and… 70

Fig. 3.4. The correlation coefficient with the inverse temperature (1/T) among individual PAH compounds. 73

Fig. 3.5. The source diagnostic ratios of particulate PAHs, (a) BaP/BghiP and (b)… 77

Fig. 3.6. The source diagnostic ratios of particulate PAHs, (a) BaA/Chry and (b)… 78

Fig. 4.1. Average size distributions of PM10 in (a) summer and (b) winter. 89

Fig. 4.2. The size distributions of PM10 and PAHs measured in W-5 in winter. 91

Fig. 4.3. Average size distribution of PAH compounds and total PAHs measured in summer. 96

Fig. 4.4. Average size distribution of individual PAH compounds and total PAHs… 97

Fig. 4.5. Air parcels movement during sampling period in (a) summer and (b) winter 98

Fig. 4.6. The source diagnostic ratios (a) BaP/BghiP, (b) Phen/Antr, (c) BaA/Chry, and (d) BaP/BaP. Typical values for the sources… 101

Fig. 5.1. Schematic diagram of knife edge surrogate surface plate (KSS) (a) Side and (b) top view 109

Fig. 5.2. Particulate PAHs air concentrations and dry deposition flukes at Seoul (S:… 116

Fig. 5.3. Average particulate (a) concentrations and (b) dry deposition fluxes of individual PAH compounds at Seoul. 117

Fig. 5.4. Overall dry deposition velocities of individual PAH compounds. 122

Fig. 6.1. Map of the sampling site (SE) and coke oven locations (PH and GY) in Korea.… 132

Fig. 6.2. Trend of the consumption for fossil fuels at Seoul (MOCIE, 2004). Petroleum… 134

Fig. 6.3. Ratio of (a) petroleum consumption by type and (b) vehicles by sector at Seoul… 136

Fig. 6.4. Consumption ratio of NG by sector at Seoul in 2003(MOCIE, 2004). 137

Fig. 6.5. Temporal trend of (a) coal, (b) petroleum, and (c) NG consumption in China,… 139

Fig. 6.6. Amounts (in PJ) and fractions (in %) of coal consumption by sector in China in… 140

Fig. 6.7. Ratio of petroleum consumption by product in (a) China and (b) Japan in 2003(BP, 2005). 141

Fig. 6.8. Estimated annual (non year specific) amounts (in Tg) and fractions (in %) of… 143

Fig. 6.9. Monthly variation of particulate PAHs concentrations at Seoul. 147

Fig. 6.10. The fraction of annual source contributions for particulate PAHs. 151

Fig. 6.11. Seasonal source contributions to particulate PAHs. 152

Fig. 6.12. Air parcels movement during sampling period in (a) spring, (b) summer, (c) fall and (b) winter. 157