摘要

本研究主要分析高屏峽谷陸棚岩心沉積物中多環芳香烴濃度隨時間分佈之情形，以探討各岩心在歷年來其多環芳香烴沉降之污染狀態及傳輸途徑，並應用化學指紋鑑識技術及統計分析方法，以瞭解岩心沉積物中多環芳香烴成份含量特徵以判斷多環芳香烴之可能污染來源。
研究結果顯示高屏峽谷陸棚岩心中Σ50 PAHs與Σ16 PAHs平均濃度分別為568~816 ng/g與169~256 ng/g，整體濃度分佈除了岩心L10與L26之外，其餘岩心在1960s~2006係以高分子量(4-6環)之多環芳香烴化合物佔優勢，而1960s以前則是以低分子量(2-3環)之多環芳香烴化合物為主。
經由群集分析(HCA)之結果，搭配化學指紋鑑識技術，可以發現南北陸棚中多環芳香烴之來源組成不太相同，南部陸棚多環芳香烴以石油及石油燃燒來源為主；而北部陸棚以石油燃燒及石油/燃燒混合性來源比例為多。
就高屏峽谷陸棚之多環芳香烴污染史而言，在1930-1950年間總多環芳香烴濃度開始呈現上升之趨勢，其可能為第二次世界大戰時大鵬灣遭受美軍猛烈的轟炸(1944年)，導致火災、沉船及洩油事件產生高含量的多環芳香烴。於1950-1990年間濃度呈現逐年增加之趨勢，可能為高屏地區重工業發展所造成。於1990-2006年間受到環保法規影響，濃度則呈現逐年下降之趨勢。但其中值得注意的是岩心L28與L29，在1990-2006年代總多環芳香烴濃度反而呈現往上升之趨勢，其可能原因是來自於高雄港疏浚淤泥棄置之關係。
本研究結果顯示北部陸棚岩心總多環芳香烴濃度明顯高於南部陸棚。與海洋沉積物品質指標進行比較，北部陸棚岩心中部分化合物濃度介於TEL到PEL之間，說明出此區域的沉積物容易對當地的底棲生物造成偶發性的影響，應加強鄰近海域的沉積物監測與管理。


中文關鍵字：多環芳香烴、高雄港、沉積物品質指標

Abstract

This study investigated the distributions of polyclic aromatic hydrocarbons (PAHs) in the sediment cores collected from continental shelf of Gaoping submarine canyon. The sediment cores were analyzed for PAHs to reconstruct historical contamination record of these compounds and to find out the possible sources, trends and fluxes.
The average concentrations of Σ50 and Σ16 PAHs ranged from 568 to 816 ng/g and from 169 to 256 ng/g, respectively. Except for sediment cores L10 and L26, the high molecular weight PAHs (4-6 ring PAHs) were found dominant in 1960s-2006, while the low molecular weight PAHs (2-3 ring PAHs) were found dominant before 1960s.
Results from diagnostic ratios and hierarchical cluster analysis (HCA) both suggested that sources of PAHs in the cores of southern continental shelf were primarily from petrogenic, while those in the cores of northern continental shelf were from pyrogenic and petroleum combustion.
There is a significant increasing of total PAH concentrations between 1930-1950, suggesting that might be an evident during the World War II. Due to increase of importing fossil fuel and the growth of heavy industrials in Gaoping area, the total concentrations of PAHs showed an increasing trend again since 1950s in the core from continental shelf of Gaoping submarine canyon. In addition, during 1990-2006, the total concentrations of PAHs showed a decreasing trend might result from the environmental protection laws. It is noteworthy that in L28 and L29 sediment cores, the increase of total PAH concentrations recorded during 1990-2006 may be due to the dumping of the sludge from dredged Kaohsiung harbor sediments.
Comparing with the sediment quality guidelines (SQG), the PAH concentrations in the northern continental shelf sediment samples were higher than the Threshold Effect Level (TEL) value, suggesting there might be an adverse biological effects caused by PAHs.


Keywords：Polycyclic aromatic hydrocarbons (PAHs), Kaohsiung harbor, Sediment quality guidelines (SQG)

目錄

謝誌
摘要
Abstract
目錄 Ⅰ
圖目錄 Ⅳ
表目錄 Ⅵ
附錄 Ⅶ
第一章 前言 1
1-1 研究動機 1
1-2 研究目的 2
第二章 文獻回顧 4
2-1 持久性有機污染物 4
2-2 多環芳香烴之物化特性 11
2-3 多環芳香烴之危害風險 15
2-4 環境中多環芳香烴之產生及來源 18
2-5 多環芳香烴之化學指紋鑑識 19
2-6 多環芳香烴之海洋沉積物品質指標 24
2-7 岩心沉積物之應用 26
2-8 研究區域—高屏陸棚 27
2-8-1 高屏峽谷與高屏陸棚之地形特徵 27
2-8-2 高屏峽谷與高屏陸棚之流場特性 28
第三章 研究方法 30
3-1 樣品之採樣與保存 30
3-2 樣品前處理 31
3-3 材料與儀器 31
3-3-1 材料 31
3-3-2 儀器設備 32
3-4 試藥及器具前處理 32
3-5 加速溶劑萃取法之原理 33
3-6 樣品分析方法 34
3-6-1 粒徑分析 34
3-6-2 總有機碳(TOC)分析 35
3-6-3 多環芳香烴分析 35
3-6-4 沉積物之定年 38
3-7 品保及品管 39
3-7-1 方法回收率 39
3-7-2 重複分析 40
3-7-3 標準查核樣品分析 40
3-7-4 方法偵測極限 42
3-8 群集分析（Hierarchical Cluster Analysis, HCA） 45
第四章 結果與討論 46
4-1 多環芳香烴之濃度隨深度之變化趨勢 46
4-2 多環芳香烴之來源性探討 56
4-3 Perylene之來源性探討 81
4-4 多環芳香烴之沉降通量（fluxes） 89
4-5 多環芳香烴污染史探討 93
4-6 總多環芳香烴濃度與總有機碳及粒徑之相關性分析 100
4-7 沉積物品質指標（Sediment Quality Guidelines, SQG） 104
4-8 國內外文獻比較 107
第五章 結論與建議 109
5-1 結論 109
5-2 建議 110
參考文獻 112
附錄 122

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