本研究針對高雄港區沉積物進行丁基錫化合物(butyltin compounds, BTs)及多環芳香烴化合物(polycyclic aromatic hydrocarbons, PAHs)之調查與污染評估。BTs調查於2006年期間採集20個沉積物樣本，PAHs調查於2006年期間採集12個沉積物樣本。分析項目包括粒徑分析、含水量、有機質(organic matter, OM)、單丁基錫(monobutyltin, MBT)、二丁基錫(dibutyltin, DBT)、三丁基錫(tributyltin, TBT)及17種PAHs含量分析，藉由監測結果評估沉積物污染程度、來源及生態環境之影響。本研究之主要目的包括：(1) 調查高雄港區沉積物BTs及PAHs之污染現況與污染來源評估。(2) 評估高雄港區沉積物BTs及PAHs對港區生態的潛在影響。(3) 提供高雄港區未來擬訂污染控制及整治方案之基礎背景資料。
研究結果顯示，高雄港沉積物BTs含量介於1.5 – 151 ng/g dry wt之間，主要以TBT為主，此顯示TBT可能因吸附機制而吸附於沉積物中。海水BTs含量介於9.7 – 270 ng/L之間，大部分測站以降解產物DBT及MBT為主，此結果顯示海水中TBT有明顯的化學或生物等降解潛能的情況。在空間分佈上，海水及沉積物中高濃度的BTs皆出現於造船廠及漁港區域，顯示船舶的相關作業(如：船舶航行、船舶維修及建造等)為港區主要貢獻BTs的來源。相關性分析顯示，海水中MBT、DBT的濃度與水溫、鹽度、溶氧及葉綠素a具有非常顯著的相關(p<0.01)，表示海水中TBT的降解受因季節變化而改變的水質參數控制。本研究監測之海水及沉積物BTs濃度皆高於可能造成生物性變異的濃度，顯示高雄港應對於TBT進行適當的管控策略。
高雄港沉積物PAHs含量介於472 – 16,201 ng/g dry wt之間，平均為5,764 ng/g dry wt，其中港區南端之工業碼頭區沉積物PAHs含量最高，其含量介於8,788 – 16,201 ng/g dry wt之間。PAHs種類組成除了工業碼頭以2到3環PAHs (42 – 37%)為主外，其餘區域主要以5到6環PAHs (42 – 71%)為主，顯示工業區的PAHs與其他區域的來源不同。另由特徵比值(diagnostic ratios)進行來源分析顯示，工業碼頭沉積物之PAHs主要由燃燒煤所貢獻，而其餘區域之沉積物PAHs來源為燃燒石油所產生。由計算沉積物PAHs之總毒性當量(toxic equivalent, TEQcarc)顯示，TEQcarc介於55 – 1,964 ng TEQ/g dry wt之間，工業區沉積物具有相對較高之潛在毒性(TEQcarc = 1,409 – 1,964 ng TEQ/g dry wt)。比較美國之沉積物品質準則(sediment quality guidelines, SQGs)顯示，工業區的PAHs含量高於低影響範圍(effects range low, ERL)，對生物的危害相對較高，而其餘區域則低於ERL，對生物產生危害的機率相對較低。
依據沉積物現場調查果顯示，港區BTs主要來自港區內之船舶相關作業(如，漁港、修造船廠)，而PAHs主要來自鄰近的工業活動，此結果將有助於高雄港建立未來污染控制及沉積物整治方案。此外，BTs及PAHs之含量皆具有潛在之生態影響，應立即採取適當的管控策略。

The distribution of butyltin compounds (BTs) in the sediments and seawater, at the river outfalls, fishing ports, shipyards, and industrial zone docks of Kaohsiung Harbor, Taiwan were investigated. Twenty sediment and seawater samples were collected from various locations in the Harbor in 2006, and analyzed for monobutyltin (MBT), dibutyltin (DBT), and tributyltin (TBT). Results showed that the concentration of total BTs varied from 1.5 to 151 ng/g in sediment samples, with TBT being the major component of the sediment samples. This suggests that sediments could be the most possible sink of TBT brought by the sorption mechanism. The concentrations of BTs ranged from 9.7 to 270 ng/L in seawater samples, whereas DBT and MBT, the degradation byproducts of TBT, were mainly the most abundant BT compounds of the seawater samples. This indicates that the abiotic or biotic degradation potential of TBT was significant. Spatially, the highest concentrations of BTs were observed in both water and sediment samples collected from the shipyard and fishing port areas. This indicates that the shipping related activities (e.g., navigation, ship repair, and ship building), would contribute most of BTs in the environment. Results show that the concentrations of degradation products (DBT and MBT) were related closely to temperature, salinity, dissolved oxygen (DO), and chlorophyll-a of the seawater. This implies that seasonal changes of the water parameters controlled the degradation of TBT in seawater. The observed levels of BT compounds in both seawater and sediments were much higher than those required to induce toxic effects on marine organisms suggesting that appropriate TBT control strategies should be taken in Kaohsiung Harbor.
Sediment samples were collected from the river outfalls, fishing ports, shipyards, and industrial zone docks of Kaohsiung Harbor, Taiwan to evaluate the distribution of polycyclic aromatic hydrocarbons (PAHs) in sediments. Collected sediment samples from 12 locations were analyzed for 17 different PAHs, organic content, and grain size. The results show that the total PAH concentrations varied from 472 to 16,201 ng/g dry wt, with a mean concentration of 5,764 ng/g dry wt The highest PAH concentrations were from the industrial zone docks situated in south Kaohsiung Harbor, ranging from 8,788 to 16,201 ng/g dry wt Among those sediment samples, the 5-, 6-ring PAHs were predominant PAH congeners in sediments, ranging from 42 to 71%. However, the dominant PAH congeners were 2-, 3-ring PAHs (37 to 42%) collected from steel industrial zone docks. This indicates that the sources for the PAH contamination at steel industrial zone docks were different from the other zones in Kaohsiung Harbor. According to the diagnostic ratios, the possible source of PAHs in the industrial zone dock could be coal combustion while in the other zones it could be petroleum combustion. The total PAH levels were expressed as the total toxic equivalent (TEQcarc). The total TEQcarc varied from 55 to 1,964 ng TEQ/g dry wt. Higher total TEQcarc values were found at industrial zone docks (from 1,404 to 1,964 ng TEQ/g dry wt). As compared with the US Sediment Quality Guidelines (SQGs), the observed levels of PAHs at industrial zone docks exceeded the effects range low (ERL), and could thus cause acute biological damage. However, the lower levels of PAHs at the other zones would not exert adverse biological effects. Results would be helpful in developing strategies for sediment remediation in Kaohsiung Harbor.

目錄
頁次
誌謝…………………………………………………………………………………... II
中文摘要………………………………………………………….............................. III
Abstract……………………………………………………………………………… V
目錄.……………………………..……………………………………........................ VII
表目錄………...………………………………………………………........................ X
圖目錄……………..…………………………………………………………………. XI
名詞說明……………………………………………………………………………... XII

第一章 前言………..………………………………..………….……....................... 1
1.1 有機錫化合物.…………………………………………………….............. 1
1.2 多環芳香烴化合物………………………………………………………… 2
1.3 研究區域……………………………………………………………........... 5
1.4 研究目的…………………………………………...……………................ 5

第二章 文獻回顧…………………………………………………………………… 6
2.1 研究區域環境背景…………………………………………………........... 6
2.1.1 高雄港地理位置………………………………………………….... 6
2.1.2 高雄港水域環境品質現況……………………………………….... 6
2.1.3 高雄港區污染源………………………………………………….... 18
2.2 OTs物化性質及在環境中的流佈與宿命………………………………….. 21
2.2.1 OTs物化性質………………………………………………………… 21
2.2.2 OTs之用途與用量…………………………………………………… 21
2.2.3 OTs進入環境的途徑………………………………………………… 24
2.2.4 OTs在水域環境中的流佈與宿命…………………………………… 27
2.2.5 OTs之生態毒性……………………………………………………… 31
2.2.6 OTs管制情形………………………………………………………… 32
2.3 PAHs物化性質及在環境中的流佈與宿命………………………………… 35
2.3.1 PAHs物化性質……………………………………………………..... 35
2.3.2 PAHs之來源……………………………………………………….... 37
2.3.3 PAHs在水域環境中的流佈與宿命………………………………... 39
2.3.4 PAHs之生態毒性…………………................................................... 40

第三章 研究材料與方法…………………………………………………………… 43
3.1 採樣點規劃……………………………………………............................... 43
3.2 樣本採集…………………………………………..……….......................... 43
3.3 實驗藥品及試劑……..…………………………………………………….. 46
3.4 樣品前處理與分析………………………………….................................... 48
3.5 品保品管控制…………………………………….………………………… 50
3.6 資料分析……………………………………………………………............ 55

第四章 結果與討論…..…………...……................................................................... 61
4.1 港區沉積物及海水BTs分佈與評估………………………....................... 61
4.1.1 沉積物BTs濃度分佈…………………………..………………….. 61
4.1.2 海水BTs濃度分佈……………….................................................... 66
4.1.3 BTs污染程度評估.............…............................................................. 71
4.1.4 BTs降解評估…………………………….…..……………............... 73
4.1.5 小結……………………………………………………….………... 74
4.2 港區沉積物PAHs分佈與評估….........……..……………………………. 77
4.2.1 PAHs濃度分佈…………………………………………................... 77
4.2.2 PAHs、OM與粒徑之相關性………………………………………... 82
4.2.3 PAHs污染來源評估………………………………........................... 84
4.2.4 沉積物潛在毒性及生物效應評估……………………….………... 87

第五章 結論與建議. ……...………….…………..…………………………………. 90
5.1 結論……………………………………………………………………....... 90
5.2 建議事項…..………………………………………………………….….... 91

參考文獻..………………………………………………............................................ 93
作者簡歷與著作…………………………………………………............................... 103

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