本研究主要分析大鵬灣灣域及外海、右岸濕地A、B區表層沉積物、紅樹林M1與M2岩心沉積物及水體(溶解態與顆粒態)中多環芳香烴含量與分佈，藉以調查研究區域內多環芳香烴污染情形，並應用化學指紋鑑定技術及統計分析，以瞭解沉積物與水中溶解態、顆粒態多環芳香烴成份含量特徵以判定其可能污染來源。
研究結果顯示沉積物總多環芳香烴(Σ51PAHs)平均濃度約介於143~1595 ng/g dw之間，水中溶解態總多環芳香烴(Σ46PAHs)之濃度為11~38 ng/L，而水中顆粒總多環芳香烴(Σ46PAHs)之濃度為1.4~15ng/L、 252~772 ng/g之間。利用沉積物品質指標(SQGs)評估沉積物之總多環芳香烴，結果大多低於沉積物品質指標之規範值，而各沉積物中可能致癌及致突變性的Benzo[a]pyrene濃度皆遠低於各項評估指標，表示此區域多環芳香烴汙染物對底棲生物無明顯之危害。而水中溶解態及顆粒態之現場分配係數(A9測站除外)高於由KOW推估之預測值，可能是受到顆粒中高分配係數的煤灰顆粒影響。
沉積物總多環芳香烴濃度與總有機碳、燃燒性多環芳香烴、黑碳及中值粒徑之相關性分析，結果為大鵬灣灣域之燃燒性多環芳香烴與總有機碳、黑碳呈現顯著相關性；而紅樹林M1與M2岩心、右岸濕地A區測站之沉積物多環芳香烴濃度與黑碳有顯著相關；水中溶解態總多環芳香烴與燃燒性多環芳香烴具有顯著相關；水中顆粒態之總多環芳香烴與燃燒性多環芳香烴及懸浮固體物呈現顯著相關性；其餘皆無顯著相關性。
透過群集分析及化學指紋鑑定之結果，大鵬灣外海以石油來源為主，大鵬灣灣域及紅樹林M1與M2岩心則主要為石油/燃燒及石油燃燒混合來源，而右岸濕地A、B區為燃燒來源為主。水體之水中溶解態及顆粒態皆傾向以石油/燃燒及石油燃燒混合來源為主。
另外各區域之Perylene的來源探討，可知大鵬灣灣域及外海沉積物主要受到生物性及某種程度的燃燒性來源影響；右岸濕地A、B區則以生物性來源為主；紅樹林M1與M2岩心之Perylene可能受到成岩作用而傾向屬於生物性來源。

The aim of this study is to investigate the distributions of polycyclic aromatic hydrocarbons (PAHs) in sediment and water (suspended particles and dissolved phase) samples collected from Dapeng Bay(coast、bay、wetland and mangrove). Chemical fingerprinting techniques and statistical analysis were applied to delineate the possible sources of PAHs in sediment and water samples.
The average concentrations of total PAHs (Σ51PAHs) ranged from 143 to 1595 ng/g dry weight (dw) in the sediments. Total PAH (Σ46PAHs) concentrations varied from 11 to 38 ng/L in dissolved phase and from 1.4 to 15ng/L (252 to 772 ng/g dw) in suspended particulate phase, respectively. Comparing with sediment quality guidelines (SQGs), the total PAH concentrations in all sediment samples were below the criteria, suggesting that no adverse biological effects would arise from the PAHs in these sediments. The partition coefficients（KOC）values of PAHs were higher than predicted values. It might be attributed to soot particles which have extremely high sorption capacities.
Total organic carbon（POC）and black carbon (BC) were significantly correlated with combustion PAH concentrations in Dapeng Bay. Combustion PAHs (Flt＋Pyr＋BaA＋Chr＋BbF＋BkFa＋BeP＋BaP＋IP＋BghiP) concentrations were significantly correlated with black carbon (BC) in mangroves sediment cores and wetland A. In addition, total PAH concentrations were significantly correlated with combustion PAHs concentrations in dissolved phase. In suspended particulate phase, total PAH concentrations and combustion PAHs concentrations were significantly correlated with suspended solid (SS).
Results from diagnostic ratios and hierarchical cluster analysis (HCA) both indicate that PAHs in the coast of Dapeng Bay were mainly from petrogenic sources, but from petrogenic and pyrogenic mixed sources in the wetland and mangrove inside the Dapeng Bay.
In addition, the origin of perylene in Dapeng Bay and coastal sediments was mainly from the biogenic and pyrogenic, while it was from biogenic origin in wetland A and wetland B. However, the origin of perylene in mangrove M1 and mangrove M2 tended to be diagenetic.

目錄
摘要
Abstract
目錄 I
圖目錄 IV
表目錄 VI
附錄頁次 VII
論文使用化合物縮寫一覽表 IX
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 3
2-3 多環芳香烴之毒理特性 4
2-4 環境中多環芳香烴傳輸途徑 5
2-5 多環芳香烴的化學指紋鑑識 9
2-6 沉積物特性與多環芳香烴之分佈 10
2-7 研究區域-大鵬灣 12
第三章 研究方法 14
3-1 採樣地點及時間 14
3-2 採樣方式 14
3-2-1 沉積物採樣方式 14
3-2-2 水樣採樣方式 14
3-3 樣品前處理 17
3-3-1 沉積物前處理 17
3-3-2 水樣前處理 17
3-4 材料與儀器 18
3-4-1 材料 18
3-4-2 儀器設備 19
3-5 試藥及器材前處理 19
3-6 分析方法 20
3-6-1 沉積物分析方法 20
3-6-2 水樣分析方法 21
3-7 儀器分析 23
3-8 品管及品保(QA/QC) 26
3-8-1 方法回收率 26
3-8-2 沉積物重複分析 26
3-8-3 空白試驗與偵測極限 26
3-8-4 標準查核樣品及添加樣品分析 28
3-9 群集分析 29
第四章 結果與討論 30
4-1 多環芳香烴之含量分析 30
4-1-1 表層沉積物及岩心多環芳香烴含量分佈 30
4-1-2 水中溶解態多環芳香烴含量分佈 36
4-1-3 水中顆粒態多環芳香烴含量分佈 38
4-2 紅樹林岩心多環芳香烴之總濃度垂直分佈趨勢 42
4-3 與全球文獻比較 45
4-3-1 沉積物多環芳香烴濃度與文獻之比較 45
4-3-2 水中溶解態多環芳香烴濃度與文獻之比較 46
4-3-3 水中顆粒態多環芳香烴濃度與文獻之比較 46
4-4 影響多環芳香烴水中顆粒態及溶解態分配之因子 50
4-5 總多環芳香烴濃度、總有機碳、黑碳及中值粒徑之相關性分析 54
4-5-1 沉積物之相關性分析 54
4-5-2 水中溶解態及顆粒態之相關性分析 57
4-6 多環芳香烴之來源判定 58
4-6-1 表層沉積物 60
4-6-2 紅樹林岩心 64
4-6-3 水中溶解態 70
4-6-4 水中顆粒態 74
4-7 沉積物Perylene之來源探討 80
第五章 結論與建議 87
5-1結論 87
5-2 建議 89
參考文獻 90
附錄 100


圖目錄
圖2-1 US EPA優先管制之16種PAHs 8
圖3-1 大鵬灣灣域及外海沉積物採樣點位置圖 15
圖3-2 右岸濕地A、B區沉積物採樣點位置圖 15
圖3-3 樣品中多環芳香烴分析流程示意圖 25
圖4-1 各區域沉積物總多環芳香烴Σ51PAHs平均濃度分佈 30
圖4-2 各區域沉積物總多環芳香烴Σ16PAHs平均濃度分佈 31
圖4-3 各區域沉積物不同環數多環芳香烴所佔百分比組成 32
圖4-4 各測站水中溶解態總多環芳香烴Σ46PAHs之濃度分佈 36
圖4-5 各測站水中溶解態總多環芳香烴Σ15PAHs之濃度分佈 37
圖4-6 各測站水中溶解態不同環數多環芳香烴所佔百分比組成 37
圖4-7 各測站水中顆粒態總多環芳香烴Σ46PAHs之濃度分佈 39
圖4-8 各測站水中顆粒態總多環芳香烴Σ15PAHs之濃度分佈 40
圖4-9 各測站水中顆粒態多環芳香烴與懸浮固體物(SS)之線性相關圖 40
圖4-10 各測站水中顆粒態不同環數多環芳香烴所佔百分比組成 41
圖4-11 各測站水中溶解態與顆粒態對多環芳香烴之貢獻 41
圖4-12 紅樹林M1岩心(a)多環芳香烴濃度及(b)不同環數與深度之關係 43
圖4-13 紅樹林M2岩心(a)多環芳香烴濃度及(b)不同環數與深度之關係 44
圖4-14 大鵬灣灣域多環芳香烴KOW與KOC關係圖 53
圖4-15 化學指紋分析鑑定理論歸納圖 59
圖4-16 大鵬灣灣域及外海、右岸濕地A、B區沉積物之HCA樹狀圖 61
圖4-17 群集分析結果沉積物各測站之地理位置圖 62
圖4-18 大鵬灣外海及灣域、右岸濕地A、B區沉積物群集分析各
Cluster PAH化合物相對濃度分佈圖 63
圖4-19 紅樹林M1與M2岩心之HCA樹狀圖 66
圖4-20 紅樹林M1與M2岩心群集分析各Cluster PAH化合物相對
濃度分佈圖 67
圖4-21 紅樹林M1岩心之PAHs污染來源化學指紋鑑定判別指標 68
圖4-22 紅樹林M2岩心之PAHs污染來源化學指紋鑑定判別指標 69
圖4-23 水中溶解態之HCA樹狀圖 71
圖4-24 水中溶解態群集分析各Cluster PAH化合物相對濃度分佈圖 72
圖4-25 水中溶解態之PAHs污染來源化學指紋鑑定判別指標 73
圖4-26 水中顆粒態之HCA樹狀圖 75
圖4-27 水中顆粒態群集分析各Cluster PAH化合物相對濃度分佈 76
圖4-28 水中顆粒態之PAHs污染來源化學指紋鑑定判別指標 77
圖4-29 相同測站之水中顆粒態與沉積物之HCA樹狀圖 78
圖4-30 水中顆粒態與沉積物之PAHs污染來源化學指紋鑑定判別指標 79
圖4-31 (a)紅樹林M1(b)紅樹林M2岩心Perylene�Σ penta-PAHs(%)之
濃度趨勢分佈圖 86


表目錄
表2-1 國際組織對PAHs毒性之研究 6
表2-2 US EPA 優先管制之16種PAHs之物化性質 7
表2-3 常見的多環芳香烴指紋鑑定 13
表3-1 各測站採樣資料 16
表3-2 各測站樣品沉積物之擬似標準品回收率 27
表3-3 各測站水中溶解態、顆粒態之擬似標準品回收率 28
表3-4 沉積物樣品重覆分析之相對差異百分比(RPD) 28
表4-1 沉積物品質指標(Sediment Quality Guidelines)與各區域PAHs
濃度比較 33
表4-2 文獻之表層沉積物及岩心中多環芳香烴濃度範圍彙整表 47
表4-3 文獻之水中溶解態中多環芳香烴濃度範圍彙整表 49
表4-4 文獻之水中顆粒態中多環芳香烴濃度範圍彙整表 50
表4-5 各測站不同化合物之logKOC值 52
表4-6 本研究之logKoc 與其他地區文獻之比較 53
表4-7 各測站沉積物之關聯係數矩陣 56
表4-8 各測站水中溶解態之關聯係數矩陣 58
表4-9 各測站水中顆粒態之關聯係數矩陣 58
表4-10 沉積物群集分析與化學指紋鑑定結果比較 70
表4-11 水中溶解、顆粒態群集分析與化學指紋鑑定結果比較 80
表4-12 文獻上海域沉積物perylene之濃度分佈彙整表 82
表4-13 各測站與燃燒性化合物(Pyr、BeP、BaP、Pery)相關係數矩陣 85


附錄頁次
附錄A-1 本研究中沉積物、水中溶解態及顆粒態分析之化合物 100
附錄B 各區域之表層沉積物測站群集分析及化學指紋鑑定結果 102
附錄B-1 大鵬灣外海沉積物之HCA樹狀圖 104
附錄B-2 大鵬灣外海沉積物群集分析各Cluster PAH化合物相對濃度
分佈圖 105
附錄B-3 大鵬灣外海沉積物之PAHs污染來源化學指紋鑑定判別指標 106
附錄B-4 大鵬灣灣域沉積物之HCA樹狀圖 107
附錄B-5 大鵬灣灣域沉積物群集分析各Cluster PAH化合物相對濃度
分佈圖 108
附錄B-6 大鵬灣灣域沉積物之PAHs污染來源化學指紋鑑定判別指標(a)Flt/(Flt+Pyr)、Ant/178(b)BaA/228、IP/(IP+BghiP) 109
附錄B-7 右岸濕地A區沉積物之HCA樹狀圖 110
附錄B-8 右岸濕地A區沉積物群集分析各Cluster PAH化合物相對
濃度分佈圖 111
附錄B-9 右岸濕地A區沉積物之PAHs污染來源化學指紋鑑定判別
指標 112
附錄B-10 右岸濕地B區沉積物之HCA樹狀圖 113
附錄B-11 右岸濕地B區沉積物群集分析各Cluster PAH化合物相對
濃度分佈 114
附錄B-12 右岸濕地B區沉積物之PAHs污染來源化學指紋鑑定判別
指標 115
附錄C-1 表層沉積物ΣPAHs之空白實驗結果與偵測極限 116
附錄C-2 水中溶解態ΣPAHs之空白實驗結果與偵測極限 119
附錄C-3 水中顆粒態ΣPAHs之空白實驗結果與偵測極限 122
附錄C-4 標準沉積物SRM 1941b多環芳香烴分析結果 125
附錄C-5 水中溶解態添加樣品回收率分析結果 126
附錄C-6 水中顆粒態添加樣品回收率分析結果 129
附錄D-1 大鵬灣外海沉積物PAHs濃度、isomer ratio、TOC、BC及
中值粒徑 132
附錄D-2 大鵬灣灣域沉積物PAHs濃度、isomer ratio、TOC、BC及
中值粒徑 134
附錄D-3 右岸濕地A區沉積物PAHs濃度、isomer ratio、TOC、BC
及中值粒徑 137
附錄D-4 右岸濕地B區沉積物PAHs濃度、isomer ratio、TOC、BC
及中值粒徑 140
附錄D-5 紅樹林M1岩心PAHs濃度、isomer ratio、TOC、BC及中值
粒徑 143
附錄D-6 紅樹林M2岩心PAHs濃度、isomer ratio、TOC、BC及中值
粒徑 146
附錄D-7 水中溶解態 PAHs濃度、isomer ratio、DOC 149
附錄D-8 水中顆粒 PAHs濃度(ng/L)、isomer ratio、SS、POC、BC 151
附錄D-9 水中顆粒 PAHs濃度(ng/g)、isomer ratio、SS、POC、BC 153

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