大氣汞研究議題已成為世界各國重視之環境焦點之一，本研究利用改良之大氣汞採樣及分析方法，從小尺度至大尺度，分別針對四種不同區域進一步量測大氣汞時空流佈、氣固相分佈、與氣象參數及法規空氣污染物相關性分析、長程傳輸途徑及與其他固定污染源汞濃度之比較。
就半導體工業園區大氣汞濃度濃度變化趨勢而言，總氣態元素汞(total gaseous elemental mercury; TGM)及顆粒態汞(particulate mercury; Hgp)濃度範圍分別介於3.30-6.89 ng/m3及0.06-0.14 ng/m3，而TGM及Hgp最高濃度分別為10.33 ng/m3及0.26 ng/m3，其氣固相分佈以TGM為主，TGM及Hgp分別介於92.59-99.01％和0.99-7.41％。整體而言，採樣期間高、低濃度之TGM分別出現於冬季及夏季，反觀Hgp則與季節變化較無相關性。此外，盛行風向扮演了影響TGM濃度高低之關鍵角色，下風處TGM濃度明顯高於上風處，此結果可說明半導體工業園區為複雜之含汞污染物排放源，亦為成為鄰近區域大氣汞濃度增加之主要原因。
就汞污染整治場址濃度變化趨勢而言，TGM及Hgp濃度範圍分別介於5.56-12.60 ng/m3及0.06-0.22 ng/m3，而落塵之汞沉降通量(deposition fluxes of dust-fall mercury; DFM)濃度範圍分別介於27.0－56.8 g/km2-month。其中，TGM和Hgp的最高濃度分別為38.95和0.58 ng/m3，其氣固相分佈則以TGM為主，TGM及Hgp分別介於97.42-99.87％和0.13-2.58％。整體而言，春季及夏季環境含汞濃度較秋季及冬季來得高，而汞污染整治場址之大氣汞排放熱點則為廢棄之氯鹼工廠，於開挖整治期間TGM最高濃度可達平均濃度之2-3倍。此外，當汞污染整治場址區域盛行方向吹南風時，對於場址北部之敏感點環境大氣汞濃度將有明顯之增加，對於敏感點之居民健康恐產生影響。
就高雄重工業都會區濃度變化趨勢而言，TGM及Hgp濃度範圍分別介於2.38-9.41 ng/m3及0.02-0.59 ng/m3，大氣汞最高濃度則分別可達9.41 ng/m3及0.59 ng/m3，其氣固相分佈則以TGM為主，TGM及Hgp分別介於92.71-99.17％及0.83-7.29％。整體而言，大氣汞濃度為乾季較濕季來得高，小港地區則為大氣汞濃度最高之區域。此外，高雄都會區大氣汞排放熱點可區分為南高雄之鋼鐵工業區及北高雄之石化工業區。
就澎湖群島沿海背景濃度變化趨勢而言，澎湖群島TGM平均濃度為3.17±1.17 ng/m3，其濃度範圍則介於1.17-8.63 ng/m3，且日間TGM濃度明顯較夜間來得高，春季為澎湖群島TGM最高之季節，夏季則接近北半球背景濃度(1.8 ng/m3)。就逆軌跡模式而言，澎湖群島TGM濃度增加，主要是受到從大陸華北地區、華東地區及中國南方之污染氣團長程傳輸之影響，而TGM平均濃度最低之夏季，則主要來自相對乾淨的南中國海，故推測量測期間之風向及污染物傳輸路徑，應為影響澎湖群島TGM濃度變化之主因。此外，就大氣汞濃度、法規空氣污染物及氣象參數相關性分析而言，TGM濃度與Hgp、SO2、NOx、CO、環境溫度及紫外線強度呈現正相關，而與O3、相對溼度及風速呈現負相關；Hgp濃度則與TGM、SO2、NOx及O3呈現正相關，而與環境溫度、相對溼度及風速呈現負相關。

The issues of atmospheric mercury have been discussed more popularly in the world. This study measured atmospheric mercury by using the modified sampling and analytical methods from four cases of small-scale regions to large-scale regions, and further investigated the tempospatial variation of atmospheric mercury, gas-particulate partition, the correlation analysis of mercury concentration with meteorological parameters and criteria air pollutants, the transportation routes of mercury, and the comparison of mercury concentration in urban areas and other stationary sources.
First of all, an one-year field measurement results at a semi-conductor manufacturing complex showed that the seasonal averaged concentrations of TGM and Hgp were in the range of 3.30-6.89 and 0.06-0.14 ng/m3, respectively, while the highest 24-hr TGM and Hgp concentrations were 10.33 and 0.26 ng/m3, respectively. Atmospheric mercury apportioned as 92.59-99.01% TGM and 0.99-7.41% Hgp. As a whole, the highest and lowest concentrations of TGM were observed in the winter and summer sampling periods, respectively, while the concentration of Hgp did not vary much seasonally. The highest TGM concentrations were always observed at the downwind sites, indicating that the semi-conductor manufacturing complex was a hot spot of mercury emission source, which caused severe atmospheric mercury contamination over the investigation region.
In an unique mercury-contaminated remediation site, an one-year field measurement results showed that the seasonal averaged concentrations of TGM and Hgp were in the range of 5.56-12.60 and 0.06-0.22 ng/m3, respectively, while the seasonal averaged deposition fluxes of dust-fall mercury were in the range of 27.0 to 56.8 g/km2-month. The maximum concentrations of TGM and Hgp were 38.95 and 0.58 ng/m3, respectively. The atmospheric mercury apportioned as 97.42-99.87% TGM and 0.13-2.58% Hgp. As a whole, the concentrations of mercury species were higher in the spring and summer than those in the winter and fall. The southern prevailing winds generally brought higher mercury concentrations, while the northern winds brought relatively lower mercury concentrations, to the nearby fishing villages. The hot spot of mercury emissions was allocated at the southern tip of the abandoned chlor-alkali manufacturing plant. On-site continuous monitoring of TGM at the mercury-contaminated remediation site observed that TGM concentrations during the open excavation period were 2 to 3 times higher than those during the non-excavation period.
In a heavily polluted industrial city, Kaohsiung, field measurement results showed that TGM and Hgp concentrations were in the range of 2.38-9.41 and 0.02-0.59 ng/m3 with the highest concentrations of 9.41 and 0.59 ng/m3, respectively. Moreover, the partition of atmospheric mercury was apportioned as 92.71-99.17% TGM and 0.83-7.29% Hgp. As a whole, the concentrations of mercury species in the dry season were higher than those in the wet season, no matter of TGM or Hgp concentration. The TGM and Hgp concentrations at Hsiao-kang site was the highest in Kaohsiung City. The hot spots of atmospheric mercury were allocated at two regions in Kaohsiung City, including a steel industrial complex in the south and a petrochemical industrial complex in the north.
In a coastal site of the Penghu Islands, the field measurement results showed that the average TGM concentration during the monitoring periods was 3.17±1.17 ng/m3 with the range of 1.17-8.63 ng/m3, as the highest concentration being observed in spring, while the average TGM concentrations in the daytime were typically higher than that at nighttime. Moreover, the lowest average TGM concentration of 1.81±0.15 ng/m3 was observed in summer. The backward trajectory simulation results showed that the elevated TGM concentrations could be transported from either North China, East China, or South China to the Penghu Islands, while those originated from South China Sea had the lowest contribution to the TGM levels of the Penghu Islands. Therefore, prevailing wind direction and air mass transportation routes potentially playing the critical roles on the variation of TGM concentration at the Penghu Islands. Furthermore, correlation analysis results indicated that the TGM concentration correlated positively with SO2, NOx, CO, ambient temperature, UVB and negatively with O3, relative humidity, and wind speed. While, Hgp correlated positively with SO2, NOx, O3 and negatively with ambient temperature, relative humidity, and wind speed.

AUTHORIZATION OF RESEARCH DISSERTATION I

ACKNOWELEDGEMENTS II

摘要 III
ABSTRACT V

TABLE OF CONTENTS VIII

LIST OF TABLES XI

LIST OF FIGUARES XIII



CHAPTER 1 INTRODUCTION 1
1.1 Background and Objectives 1
1.2 Structure and Scope 5
CHAPTER 2 REVIEW OF LITERATURES 10
2.1 Physicochemical Characteristics of Mercury 10
2.2 Speciation and Composition of Atmospheric Mercury in Ambient Air 12
2.3 Sources, Transformation, and Cycle of Atmospheric Mercury 14
2.4 Health Effects of Atmospheric Mercury 21
2.5 Overview of Atmospheric Mercury Researches 25
CHAPTER 3 RESEARCH APPROACHES 33
3.1 Overview of the Measurement Methods for Atmospheric Mercury 33
3.2 Improvement of the methods for TGM and Hgp Measurement 37
3.3 Instrumental and Model Analysis 45
CHAPTER 4 TEMPOSPATIAL VARIATION OF ATMOSPHERIC MERCURY AND ITS GAS-PARTICULATE PARTITION IN THE VICINITY OF A SEMI-CONDUCTOR MANUFACTURING COMPLEX 50
4.1 Introduction 50
4.2 Selection and Description of Sampling Sites 51
4.3 Partition of TGM and Hgp 51
4.4 Seasonal Variation of TGM and Hgp 54
4.5 Spatial Distribution of TGM and Hgp 56
CHAPTER 5 PARTITION AND TEMPOSPATIAL VARIATION OF GASEOUS AND PARTICULATE MERCURY AT A MERCURY-CONTAMINATED REMEDIATION SITE 63
5.1 Introduction 63
5.2 Selection and Description of Sampling Sites 64
5.3 Seasonal Variation and Partition of TGM and Hgp 66
5.4 Spatial Distribution of TGM and Hgp 71
5.5 Hourly Variation of Mercury Emission from Open Excavation 74
5.6 Deposition Flux of Wet/Dry Mercury 76
CHAPTER 6 TEMPOSPATIAL VARIATION AND PARTITION OF ATMOSPHERIC MERCURY IN AMBIENT AIR OF AN INDUSTRIAL CITY 79
6.1 Introduction 79
6.2 Selection and Description of Sampling Sites 80
6.3 Seasonal Variation and Partition of TGM and Hgp 81
6.4 Spatial Distribution of TGM and Hgp 87
CHAPTER 7 MEASUREMENT OF TOTAL GASEOUS MERCURY AT THE MARINE BOUNDARY LAYER AND THE ASSOCIATED LONG-RANGE TRANSPORTIATION 90
7.1 Introduction 90
7.2 Selection and Description of Monitoring Sites 91
7.3 Seasonal and Daily Variation of TGM Concentration 94
7.4 Hourly Variation of TGM Concentration 98
7.5 Transportation Routes of TGM toward the Penghu Islands 100
CHAPTER 8 COMPARISON OF MERCURY LEVELS AND CORRELATION ANALYSIS 110
8.1 Comparison of TGM and Hgp Levels with Other Stationary Sources 110
8.2 Comparison of TGM and Hgp Concentrations with Major Cities of Taiwan and Other Countries 113
8.3 Correlation of TGM with Meteorological Parameters and Criteria Air Pollutants 117
CHAPTER 9 CONCLUSIONS AND SUGGESTIONS 120
9.1 Conclusions 120
9.2 Suggestions 124
REFERENCES 126
APPENDIX A Calibration Curves of Gaseous and Particulate Mercury A-1
APPENDIX B Chemical Analytical Data of Manual and Auto Mercury Monitoring B-1

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