本論文主要目的是研究季節與傳輸路徑，對大氣中微粒化學特徵的影響及東亞沙塵暴大氣微粒金屬指標。前段部分，探討台灣西部海岸地區PM2.5與PM2.5-10微粒上金屬季節性變化與傳輸路徑之化學特徵。微粒採樣從2009年3月到2010年2月，以ICP及ICP-MS分析PM2.5及PM2.5-10中16個金屬元素。多種方法、逆軌跡分析、富集因子與主成分分析用來鑑定微粒上金屬元素可能來源。PM2.5與PM2.5-10年平均質量濃度分別是34.9±20.6及20.8±11.3 μg m-3。PM2.5及PM2.5-10微量金屬最高值濃度出現在冬季，PM2.5-10上主要金屬元素最高值則出現在秋季。富集因子結果顯示PM2.5及PM2.5-10上的銅、砷、鋅、鉛、鎘及硒為人為來源。主成分分析結果顯示，來自當地及鄰近地區的交通、煤及重油燃燒為研究地區主要的人為來源。逆軌跡分析顯示來自大陸的東北季風 (冬季) 展現與來自東南亞地區的西南季風 (夏季) 有不同的化學特徵。值得注意，即時在相同季節，不同的長程傳輸路徑，會影響微粒上金屬濃度及與金屬相關的總過量致癌風險。
2010年2月至3月東亞沙塵暴期間，在台灣南部研究大氣中粒狀物及18種金屬元素，在四種顆粒相的變異性。PM2.5、PM2.5-10、PM10及TSP四種顆粒相平均質量濃度變化，在亞洲沙塵暴期間以PM2.5-10為主，非沙塵暴期間則以PM2.5 為主。地殼元素 (鐵、鎂、鍶、鈷、鋇及錳)於亞洲沙塵暴及非沙塵暴期間展現明顯的差異，故這些元素可用來當作沙塵暴入侵指標；除了鈣及鋁元素外。在微粒質量及金屬濃度變化，PM2.5-10顆粒相可以清楚區分出亞洲沙塵暴及非沙塵暴。富集因子顯示大部分人為金屬元素，在沙塵暴期間明顯低於非沙塵暴期間。此外，粗顆粒相的人為金屬元素富集因子也可做為沙塵暴入侵指標。除了傳輸路徑外，沙塵暴對受體影響的程度和滯留時間也有相關。

The main goal of this dissertation was to investigate the effect of seasonality and transport route on chemical characteristics and marks of East Asian dust storms in ambient particulate matter. In first part, this study investigated seasonal variations and transport route in PM2.5 and PM2.5-10 associated metallic elements in the western coastal area of southern Taiwan. Particle sampling was conducted from March 2009 to February 2010. Sixteen metallic elements in PM2.5 and PM2.5-10 were determined by ICP and ICP-MS. Multiple approaches, backward trajectory analysis, enrichment factor (EFc), and principal component analysis (PCA), were used to identify the potential sources of the metallic elements. The annual mean concentrations of PM2.5 and PM2.5-10 were 34.9±20.6 and 20.8±11.3 μg m-3, respectively. Analysis of the temporal distribution revealed seasonal peaks for most of the trace elements in PM2.5 and PM2.5-10 during winter season and the major elements in PM2.5-10 during the autumn season. EFc results confirmed that the main contributors of Cu, As, Zn, Pb, Cd, and Se were anthropogenic sources in PM2.5 and PM2.5-10. PCA identified traffic emissions, coal, and heavy oil combustion from both local and neighboring areas, as the major anthropogenic sourcesin the sampling site. With backward trajectory analysis, northeast monsoon (winter) originated from China demonstrated different chemical characteristics from those of southwest monsoon (summer) from the Southeast Asian countries. It is noted that even in the same season, route-dependent effects of long-range transport in metallic concentrations and total excess cancer risk (ECR) of health-related metals were observed.
In the mark study of East Asian dust storms, the variationsin particulate matter (PM) and in eighteen metallic elements in four different particle sizes in the air of southern Taiwan were investigated from February to March 2010. The variation inmean mass concentrations of PM2.5, PM2.5-10, PM10, and TSP between Asian dust storm (ADS) and non-dust storm (NDS) periods suggested that the dominant fractions were PM2.5-10 and PM2.5, respectively. The obvious differences in metallic element concentrations between ADS and NDS periods suggested that crustal elements (Fe, Mg, Sr, Co, Ba and Mn) can be used as dust storm indicators, in addition to Ca and Al. Both mass fractions and metallic concentration ratios indicated that the PM2.5-10 fraction can distinguish between ADS and NDS periods. An enrichment factor (EFc) demonstrated that most anthropogenic elements were significantly lower in ADS periods than in NDS periods. The EFc values for anthropogenic elements in coarse particles may be used as indicators of dust storm invasion as well. An association was found between the extent of dust storm effects on receptors and the residence time (duration) of the event, in addition to the transport pathway.

TABLE OF CONTENTS

ACKNOWLEDGEMENTS…………………………………….……….…… i
摘要……………………………………………………………..………………iii
ABSTRACT………………..………………………………………………...…iv
TABLE OF CONTENTS…………..………………………………….……….vii
LIST OF TABLES……………………..…………………………….….……..x
LIST OF FIGURES………………………..…………………………………..xii

CHAPTER 1 INTRODUCTIONS………………………………………...….1

1.1 Background of the study………………………………………………….…1

1.2 The aim of this dissertation……………………………………………....…3

CHAPTER 2 LITERATURE REVIEW………………………….……..……5

2.1 Particle characteristics…………………………………………….…..…….5

2.1.1 Particle size distributions…..……………………………..…….……....5

2.1.2 Particles and human health……………..……………………….……....6

2.2 Source identification……………………………………………….…….…..7

2.3 Previous studies in Taiwan……………………………………………...…...7

2.4 Dust storm……………………………………………………………..…..…8

2.4.1 Dust storm sources…..………………………………………………..…9

2.4.2The effects of dust storm on human health and the environment…....….10

2.4.3Dust storm chemical characteristics……….…………..…………..….11

Chapter 3 MATERIALS AND METHODS……………….……………..…16

3.1 Sampling site………………………………………………………………16

3.2 Sampling and analytical procedures…………………………………..…..16

3.3 Enrichment factors…………………………………….…………………..19

3.4 Principal component analysis…………………....…..….…………….......20

3.5 Excess cancer risk…….…………………………….….………….……....20

3.6 Quality control and quality assurance…………………….…………….....21

Chapter 4 RESULTS AND DISCUSSION………………………………..…26

4.1The effects of seasonality and transport route…………………….…….….26

4.1.1 Meteorological conditions……………………………………..….......26

4.1.2 Particle mass concentrations and size fraction ratios………….……...26

4.1.3 Concentration of metallic elements……………………………….…...29

4.1.4 Source identification by enrichment factors……….……………….....32

4.1.5 Source apportionment by principal component analysis .……….....…33

4.1.6 Backward trajectory analysis………………………………….…….....35

4.1.7 Excess cancer risk assessment in PM2.5 and PM2.5-10……………...…..40

4.2 Markers of East Asian dust storms……………………………………....….56

4.2.1 Identification of dust storm events………………………………….….56

4.2.2 Aluminum element in PM10…………………………………………….56

4.2.3 Temporal variations of PM10 concentrations…………………………...57

4.2.4 Particle mass concentrations and size fraction ratios…………………..60

4.2.5 Concentration of metallic elements……………………………..……...62

4.2.6 Enrichment factors assessment..…………………………..……….…...64

4.2.7 Spatial variations during a severe dust storm event……………….……65

Chapter 5 CONCLUSIONS AND RECOMMENDATIONS……………......79

5.1 Conclusions……………………………………………….……………..…..79

5.1.1The effects of seasonality and transport route…………….………….....79

5.1.2 Markers of East Asian dust storms…………………………….….…….80

5.2 Recommendations…………………………………….…………….….....81

REFERENCES………………………………………………..…………….….84

APPENDIX A SRM 1648a analytical result and seasonalconcentrations of
PM2.5 and PM2.5-10 in the air……………………………........108

APPENDIX B The results of quality samples and elemental
concentration (ng m-3) in all PM2.5, PM2.5-10, PM10,
and TSP samples during the NDS and ADS periods………...113

LIST OF PUBLICATION…………………………...………………..………..118

CONFERENCE…………………………………………………………..…….118



LIST OF TABLES
Table 3-1. Results of accuracy and precision of duplicate, quality control,
spike samples, SRM1648a recovery, and method detection limits
in seasonal study………...........................................................25

Table 4-1. Atmospheric particulate mass concentrations (μgm-3) in this study….49

Table 4-2. Seasonal concentrations of PM2.5 and PM2.5-10 metallic elements in air
at the sampling site…………………………………………….50

Table 4-3. PCA factor loadings for metallic elements in PM2.5 and PM2.5-10 during
the sampling period…………………………………………...51

Table 4-4. The mean concentrations (ng m-3) of PM2.5 and PM2.5-10 in the sampling
site under different air masses…………………………………..52

Table 4-5. Comparison of selected PM2.5-bounded metallic elements average concentrations in the Southeast Asian countries…………………..53

Table 4-6. The mean (SD) EFc of PM2.5 in the sampling site under different air masses………………………………………….…………....54

Table 4-7.Seasonal excess cancer risk of carcinogenic metals in PM2.5 and
PM2.5-10……………………………………………………..…55

Table 4-8. Ambient PM concentrations (µg m-3) and ratios in the southern coastal
area of Taiwan during the sampling periods…………………..…..75

Table 4-9. Elemental concentrations (ng m-3) in PM2.5, PM2.5-10, PM10, and
TSP during the NDS and ADS periods………………………..….76

Table 4-10. Calcium concentrations obtained from routes of northeastern (NE)
and north (N) China in PM2.5, PM2.5-10, PM10 and TSP during
ADS periods……………………………………………….....77

Table.4-11.Comparison of metallic concentrations in aerosol collected in
Kaohsiung, Hengchun, Xiamen and Gwangju during the severe
ADS period(March 19-23), 2010…………………………….....78


















LIST OF FIGURES
Figure 2-1.Typical PM mass showing the multimodal nature of the ambient
aerosol. Figure extracted from Lighty (2000)………………….14

Figure 2-2.Primary sources of desert dust and their atmospheric pathways
around the world. (1) African desert dust is transportedacross
the Atlantic to the northern Caribbean and North America.
(2) African desert dust is transported across the Atlantic to the
southern Caribbeanand South America. (3) The Asian dust
season typically lasts from late February to late April. (4)
Large Asian dust events can travel significantdistances in
the Northern Hemisphere. Yellow lines show Asian desert
dust atmospheric routes, orange lines show African dust routes,
brown linesshow routes of other desert dust sources, and broken
black lines depict wind patterns. Figure extracted from
Griffin (2007)………………………………………………15

Figure 3-1.Map of the sampling site, located on the campus of National
Sun Yat-sen University, Kaohsiung…………………………….23

Figure 3-2. The ambient aerosol samplers in this study……………………...24

Figure 4-1. Wind rose during the study period……………………………...42

Figure 4-2. Correlation between PM2.5 and PM10 in the sampling site…………43

Figure 4-3. Seasonal metallic element distributions of PM2.5 (F) and PM2.5-10 (C)
in PM10…………………………………………………..…44

Figure 4-4. Seasonal enrichment factors of elements in PM2.5 and PM2.5-10……..45

Figure 4-5. Principle component score plot of PM2.5 size for metallic elements in
thesampling site……………………………………………..46

Figure 4-6. Backward trajectories of air masses during summer (SR1 and SR2)
and winter (WR1, WR2 and WR3) (a) originated from the sea and
passed through the Philippines,(b) originated from the sea, (c) north
and northeast regions through the inland areas and coastal China, (d) northeast regions through theShandong Peninsula and outflowed to
the sea, and (e) through the Philippines and marine regions………47

Figure 4-7. Excess cancer risk of carcinogenic metals in PM2.5 and PM2.5-10
arising from different transport routes………………………….48

Figure 4-8. The filter samplers during East Asian dust storm (left) and
Non-dust storm (right) periods………………………………….69

Figure 4-9. Aluminum concentration in PM10 during the sampling campaign…...70

Figure 4-10. Daily variations of PM10 concentrations at different air monitoring
stations in (a) Eastern Asia and (b) Taiwan during the period of a
severe dust storm (March 2010)………………………………..71

Figure 4-11. ADS/NDS elemental concentration ratios in PM2.5, PM2.5-10, PM10, and TSP…………………………………………………………72

Figure 4-12. Asian Dust Storm backward trajectories on March 16 (a)
(northeastern China) and March 21 (b) (north China) in 2010……...73

Figure 4-13. Average enrichment factors of metallic elements in (a) PM2.5,
(b) PM2.5-10, (c) PM10 and (d) TSP during NDS and ADS periods.
(Blank on the top of bar : no significant difference; *: t-test, P<0.05;
**: t-test, P<0.01)……………………………………………..74

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