多環芳香烴(polycylic aromatic hydrocarbons, PAHs)為環境中常見之有機污染物，因其疏水性使多環芳香烴於水中易吸附於懸浮顆粒上，本研究主要分析台灣高屏海域水中懸浮顆粒之多環芳香烴含量分佈情形，並利用化學指紋鑑定(chemical fingerprinting)、主成分分析(principal component analysis, PCA)及群集分析(hierarchical cluster analysis, HCA)辨別多環芳香烴之組成特徵，探討高屏海域之懸浮顆粒可能來源。
研究結果顯示四次採樣高屏海域顆粒相多環芳香烴總濃度(sum of 36 PAH compounds)介於0.20~34.4 ng/L，平均2.53±2.19 ng/L。本研究區域以高屏峽谷之測站多環芳香烴總濃度有較高之趨勢(四季平均3.88±3.92 ng/L)。2012年11月受到高屏峽谷多環芳香烴總濃度高值影響，使該月份於四次採樣中有較高平均濃度4.42±8.64 ng/L(0.20~34.4 ng/L)。懸浮顆粒濃度轉換所得懸浮顆粒上多環芳香烴含量(ng/g)，四次採樣濃度介於137~4270 ng/g，平均為1010±825 ng/g，懸浮顆粒上多環芳香烴含量以2013年3月較高。各區域懸浮顆粒上多環芳香烴含量分別為近岸區域507±204 ng/g、高屏峽谷591±415 ng/g及外海測站617±381 ng/g，外海測站懸浮顆粒上多環芳香烴含量有略高於其他區域之情形，可能是因為高屏海域離岸愈遠懸浮顆粒粒徑愈小，其比表面積愈大容易吸附更多有機污染物所造成。高屏海域之多環芳香烴總濃度與國外文獻比較，屬於低污染範圍。
由化學指紋分析、主成分分析及群集分析結果顯示2012年5月及11月高屏海域懸浮顆粒來源較偏向石油性及石油性燃燒，2012年9月則偏向石油性燃燒及燃燒性，而2013年3月偏向燃燒性來源。以區域來看，高屏峽谷及高屏外海測站底層主要偏向石油性來源，高屏峽谷可能因峽谷內海流以沿峽谷進出之潮汐流為主，使其不易受其他區域影響，高屏海域表層懸浮顆粒來源受季節變化影響，但於近岸區域則受人為污染影響，有較強烈燃燒性訊號。

This study determined the distribution of particulate polycyclic aromatic hydrocarbons (PAHs) in Gaoping coastal area. In addition, principal component analysis (PCA), hierarchical cluster analysis (HCA) and chemical fingerprinting were performed to investigate the possible sources of PAHs in this area.
The total concentrations of 36 analyzed PAHs (ΣPAHs) varied from 0.20 to 34.4 ng/L in the water column with the mean value of 2.53±2.19 ng/L. Higher ΣPAHs values were observed in Gaoping Submarine Canyon in November 2012 due to the higher contents of suspended particles. ΣPAHs on suspended particles varied from 137 to 4270 ng/g with the mean value of 1010±825 ng/g. Higher values occurred at stations W05, W07, W08, W10 and W11 whose particles were finer and bearing higher sorption capacity in general. In addition, PAH concentrations were found significantly correlated with organic carbon content (R=0.30, P<0.05). Relatively, particulate PAH concentrations in Gaoping coastal area were at lower level comparing with other areas in the world.
Results from chemical fingerprinting, HCA and PCA indicate that particulate PAHs in the study area were mainly from petrogenic sources and petroleum combustion in May and November 2012, from petroleum combustion and pyrogenic sources in September 2012; while from pyrogenic sources in March 2013. The characteristics of bottom suspended particles in Gaoping Submarine Canyon were different from other samples. The tidal current in the canyon might cause those particles distinct from other areas in source recognition. In addition, the surface particles exhibited stronger signal from terrestrial input and atmosphere deposition.

目錄
摘要 i
圖目錄 vi
表目錄 viii
附錄目錄 viii
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 3
2.1 多環芳香烴之特性 3
2.2 多環芳香烴之來源 6
2.3 多環芳香烴之化學指紋鑑定 7
2.4 水中懸浮顆粒與疏水性有機污染物分佈 8
2.5 研究區域背景 9
第三章 研究方法 10
3.1 材料與儀器 10
3.1.1 材料 10
3.1.2 儀器 11
3.2 試藥及器具前處理 11
3.3 採樣與保存 12
3.4 分析方法 14
3.4.1 樣品前處理 14
3.4.2 樣品定量 16
3.5 品管與品保 (QA/QC) 17
3.5.1 方法回收率 17
3.5.2 實驗空白分析 17
3.5.3 方法偵測極限 17
3.6 群集分析 (hierarchical cluster analysis, HCA ) 18
3.7 主成分分析(principal components analysis, PCA) 18
第四章 結果與討論 19
4.1 顆粒相多環芳香烴 19
4.1.1 顆粒相多環芳香烴濃度分佈 19
4.1.2 多環芳香烴環數百分比分佈 27
4.1.3 多環芳香烴與有機碳相關性分析 31
4.2 文獻比較 32
4.3 化學指紋分析 35
4.3.1 四季化學指紋分析 35
4.3.2 各季化學指紋分析 40
4.4 統計分析 43
4.4.1 主成分分析 43
4.4.2 群集分析 48
4.4.3 各月份統計分析 53
4.5 Perylene 來源探討 82
第五章 結論與建議 85
5.1 結論 85
5.2 建議 87
參考文獻 88
附錄 93

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