海水表面薄層(sea-surface microlayer, SML)，由於本身特殊組成使得污染物相對於表層水(sub-surface water, SSW)呈現明顯累積，且對於海洋環境中有機污染物的傳輸與宿命扮演很重要的角色。但目前對於污染物在SML的蓄積特性及與環境因子的相關性尚未有完整研究。第二章首先在高雄地區對界面活性劑(surfactant)在SML與SSW之間的濃度與蓄積特性進行調查，同時與馬來西亞樣品比較，探討來源與人為活動對於界面活性劑分佈及與水體物化特徵的相關性。結果發現陰離子界面活性劑(MBAS)為主要貢獻，且其濃度呈現高雄高於馬來西亞。因高雄位於工業區，人為污染排放中包含了大量界面活性劑；相較於主要是農業活動的馬來西亞而言，高雄有較高的環境風險。高雄測站的溶解性有機碳(dissolved organic carbon, DOC)及陰、陽離子界面活性劑(MBAS和DBAS)濃度在SML和SSW中呈現明顯相關，表示有強烈的水體交換。且高雄區域的界面活性劑濃度分佈受到DOC與鹽水稀釋作用影響。
第三章，我們探討持久性有機污染物中的多環芳香烴(polycyclic aromatic hydrocarbons, PAHs)與多氯聯苯(polychlorinated biphenyls, PCBs)在空間分佈情形、來源、蓄積特性及毒性評估；並探討污染物與水體特性之相關性。結果顯示SML中污染物濃度高於SSW，且約80%污染物集中於顆粒態。根據相關性分析，僅DOC含量與部份污染物濃度有顯著相關。而低環數PAHs濃度則與水溫有顯著正相關。本研究中污染物的富集係數(enrichment factor, EF)大於1，顯示污染物蓄積於SML。由化學指紋鑑定及主成份分析顯示，高雄研究區域中PAHs傾向高溫燃燒及石化產物的排放的混合來源，與過往該區域結果相似。依沉積物品質參考準則(Sediment Quality Guidelines, SQGs)，總顆粒相PAHs濃度大部分低於標準值，但部分PAHs化合物則高於相對的ERL(effect range-low)值。總顆粒相PCBs濃度範圍大多介於ERL與ERM(effect range-media)間，顯示其環境中生物可能受到部分影響。最後在第四章，藉批次動力學實驗，敘述人工海水表面薄層對污染物naphthalene (Nap)、anthracene (Ant)、phenanthrene (Phe)、fluoranthene (Flt) 及 pyrene (Pyr)的分佈特性。由動力學實驗結果，PAHs達到平衡時間的快慢與其疏水特性有很大的相關性。而在現場樣品部份，疏水性越強的污染物與其分配係數(KD, distribution coefficient)呈現相反趨勢。

The sea-surface microlayer (SML) is markedly different in characteristics when compared with the sub-surface water (SSW) and plays an important role of the fate and transport of organic pollutants. However there have few studies reporting the enrichment behavior and relationship with water parameter of contaminants in the SML. In chapter 2, samples of SML and SSW were collected from two areas-Kaohsiung City and the southwest coast of Peninsular Malaysia to study the influence of SML on enrichment and distribution and to compare with the SSW. Anionic surfactants (MBAS) predominated in this study and were significantly higher in Kaohsiung than in Malaysia. Industrial areas in Kaohsiung were enriched with high loads of anthropogenic sources, accounted for higher surfactant amounts than in Malaysia, where pollutants were associated with agricultural activities. The dissolved organic carbon (DOC), MBAS, and cationic surfactant (DBAS) concentrations in the SML correlated to the SSW, reflecting water exchanges in Kaohsiung. The relationships between surfactants and the physiochemical parameters indicated that DOC and saltwater dilution might affect the distributions of surfactants in Kaohsiung. In Malaysia, DOC might be the important factor controlling DBAS. In chapter 3, selected polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) of the SML and SSW were analyzed to determine the occurrence and distribution in Kaohsiung Harbor and adjacent area. PAH and PCB concentrations in the SML were higher than those in the SSW. Overall, the particulate pollutants were all higher than those of dissolved pollutants. Correlation analysis showed significant relationships between DOC and the concentrations of total PAH, particulate PAH, and dissolved PCB. The mean enrichment factors (EFs) of PAHs and PCBs were higher than 1, indicating the enrichment in the SML. Moreover, isomer ratio and principal cluster analysis (PCA) showed the dominance of mixing petroleum and combustion source, which similar to the previous results in this area. Total particulate PAHs at most sites are below the toxicity thresholds, with a few individual PAHs between the ERL (effect range-low) and ERM (effect range-median) values. Most total particulate PCB concentrations were between ERL and ERM values indicating a potential biological impact. Finally in chapter 4, batch experiments were conducted to study the distribution behaviors between the artificial SML and PAH, including naphthalene (Nap), anthracene (Ant), phenanthrene (Phe), pyrene (Pyr) and fluoranthene (Flt). The results showed that the higher hydrophobic the PAH are, the quicker the equilibriums achieve. KD (distribution coefficient) was determined for five PAH compounds of the field sample and showed the opposite trend of decreasing KD with increasing polarity.

謝誌 ............................................................................................................i
摘要 ...........................................................................................................ii
Abstract ........................................................................................................iv
Table of Content ........................................................................................vi
List of Figures ............................................................................................x
List of Tables ...........................................................................................xiii
Chapter 1 Introduction ..................................................................................1
1.1 The sea-surface microlayer .....................................................................1
1.2 Surfactant basic information ...................................................................4
1.3 Two classes of persistent organic pollutants: polycyclic aromatic hydrocarbons and polychlorinated biphenyls .....................................................................................7
1.3.1 Polycyclic aromatic hydrocarbons (PAHs) ......................................................7
1.3.2 Polychlorinated biphenyls (PCBs) ................................................................10
1.4 Overview of Kaohsiung Harbor ...............................................................................13
1.5 Objectives .................................................................................................................15
Chapter 2 Surfactants in the sea-surface microlayer and sub-surface water at estuarine locations: their concentration, distribution, enrichment and relation to physicochemical characteristics ................................................16
2.1 Background ....................................................................................................16
2.2 Material and Methods ......................................................................................17
2.2.1 Study area and sampling .............................................................................17
2.2.2 Surfactant analysis .....................................................................................20
2.2.3 Quality assurance and quality control .............................................................21
2.2.4 Statistical Analysis.........................................................................................22
2.3 Results and Discussion ....................................................................................24
2.3.1 Distributions of the surfactants in the SML and SSW .....................................24
2.3.2 Relationship with the bulk parameters of water ...........................................32
2.3.3 The enrichment in the SML ........................................................................37
2.4 Summary ........................................................................................................40
Chapter 3 Enrichment of polycyclic aromatic hydrocarbons and polychlorinated biphenyls of the sea-surface microlayer in Kaohsiung Harbor and adjacent area ........................41
3.1 Background ....................................................................................................41
3.2 Material and Methods .......................................................................................42
3.2.1 Chemicals .................................................................................................42
3.2.2 Sampling and preparation ............................................................................43
3.2.3 Analytical procedures ..............................................................................47
3.2.4 Quality assurance and quality control ........................................................48
3.3 Results and Discussion ....................................................................................49
3.3.1 Level and distribution of SML and SSW PAHs ..............................................49
3.3.2 Concentration and distribution of PCBs in the SML and SSW .......................61
3.3.3 Correlation of PAHs and PCBs with physicochemical parameters .................70
3.3.4 Enrichment in the SML of the PAHs and PCBs..............................................72
3.3.5 Pollutant sources of PAHs ..........................................................................78
3.3.6 Toxicity assessment .....................................................................................84
3.4 Summary ........................................................................................................90
Chapter 4 Determinate the distribution coefficient of polycyclic aromatic hydrocarbons in multiple artificial sea-surface microlayer by fluorescence quenching method……........91
4.1 Background .....................................................................................................91
42 Material and Methods ........................................................................................92
4.2.1 Chemicals and reagents ............................................................................92
4.2.2 Batch distribution experiments ..................................................................93
4.2.3 The calculation of distribution rate constant (k) .........................................95
4.3 Results and Discussion ....................................................................................96
4.3.1 Select conditions of the batch distribution experiment ...................................96
4.3.2 Assessment of the distribution coefficient (KD) with multiple artificial SML and
application to environmental water samples ........................................................101
4.4 Summary .......................................................................................................109
Chapter 5 Conclusions and Suggestions ...................................................111
5.1 Conclusions ...................................................................................................111
5.2 Suggestions for future works ...........................................................................112
References ..........................................................................................................114
Author’s curriculum vitae .....................................................................................131

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