臺灣博碩士論文加值系統

本研究主要初步調查花蓮和平港與和平溪溪口沈積物中多環芳香烴和多氯聯苯的含量、分佈與特性，比較和平港內與港外（溪口）沈積物中多環芳香烴和多氯聯苯含量與分佈，以化學指紋鑑識技術及統計方法分析沉積物中多環芳香烴成份，並探討其可能之來源。
研究結果發現，花蓮和平港與和平溪溪口沈積物的總多環芳香烴和總多氯聯苯濃度分佈介於 8∼312 ng/g dw和 7∼567 ng/g dw之間。在空間上的分佈，和平港內總多環芳香烴和總多氯聯苯濃度比港外高，和平溪口遠低於和平港之含量。和平溪口的沈積物的多環芳香烴和多氯聯苯四季變化不大。
Naphthalene、 Phenanthrene、 Fluoranthene、 Pyrene、 Benzo(a)anthracene、Chrysene及Benzo(b)fluoranthene為和平港沈積物中多環芳香烴化合物的優勢物種。而和平溪口的多環芳香烴化合物的優勢物種為Naphthalene。和平港及和平溪口沈積物中總多環芳香烴含量屬於低污染區。與海洋沈積物品質參考標準相較，此地區多環芳香烴對底棲生物的影響不大。依主成份分析（PCA）及多環芳香烴異構物指紋分析結果明顯區分出兩個群集（Group1及Group2）。Group1為和平港沈積物多環芳香烴，大部分以燃燒為主要來源，尤其是煤燃燒；少部分石油來源的多環芳香烴，可能是船隻溢油的意外污染事件沈降而來。Group2屬於和平溪溪口沈積物多環芳香烴，以低分子量佔較多比例，主要來源傾向石油來源。
總多氯聯苯含量與國內外文獻比較，和平港受多氯聯苯污染程度屬較低。與多氯聯苯的海洋沈積物品質參考標準相較，和平港港內（採樣點A站及B站）為會對海洋生物造成影響的棲地，港外（C站）為對海洋生物有偶發性的影響，而和平溪口（D站）屬於對底棲生物有害影響不大的棲地。

Surface sediment samples were collected in the He-Ping Harbor and Estuary, Hualien, between October 2005 and August 2006, to examine spatial and temporal variability in polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) concentrations. The sum of the 16 USEPA priority pollutant PAHs varied from 8 to 312 ng g-1 dry wt. Concentrations of PCBs in the sediments varied widely, ranging from 7 to 567 ng g-1 dry wt. The spatial distribution of PAH and PCB concentrations in He-Ping Harbor was higher than that in He-Ping Estuary.
Naphthalene, Phenanthrene, Fluoranthene, Pyrene, Benzo(a)anthracene, Chrysene and Benzo(b)fluoranthene were the dominant PAHs found in the He-Ping Harbor sediments. The dominant PAH in He-Ping Estuary was Naphthalene. The PAH contamination of sediments from Hualien He-Ping Harbor and He-Ping Estuary was relatively low compared to other studies. In comparison with sediment quality guidelines (SQGs), the PAH concentrations of all sediment samples were lower than those outlined in the criteria, which suggests no evident adverse biological effects due to PAHs.
Principal component analysis (PCA) revealed that PAHs can be classified into two groups. In addition, according to molecular indices based on isomeric PAH ratios, pollution sources of each group can be specified. Group 1, in stations located in He-Ping Harbor, has mainly pyrogenic contamination sources. Group 2 belongs to He-Ping Estuary, which has mainly petrogenic sources.
To compare with studies in other countries, the PCB pollution of sediments in He-Ping Harbor falls near the median. To compare with sediment quality guidelines (SQGs), the PCB concentrations in He-Ping Harbor were also in the middle, which is evident of adverse biological effects. PCBs in He-Ping Estuary represent a minimal-effects toxic range.

口試委員會審定書………………………………………………i
中文摘要…………………………………………………………ii
英文摘要…………………………………………………………iii
目錄………………………………………………………………v
表目錄………………………………………………………………viii
圖目錄………………………………………………………………x
第一章 前言………………………………………………………………1
1.1 研究緣起………………………………………………………1
1.2 研究目的………………………………………………………2
第二章 文獻回顧…………………………………………………………3
2.1 疏水性有機污染物……………………………………………3
2.2 多環芳香烴概述………………………………………………4
2.2.1 多環芳香烴之研究沿起………………………………4
2.2.2 多環芳香烴之形成機制………………………………5
2.2.3 多環芳香烴之特性……………………………………6
2.2.4 多環芳香烴之危害……………………………………6
2.2.5 多環芳香烴之化學指紋分析…………………………7
2.3 多氯聯苯概述…………………………………………………8
2.3.1 多氯聯苯之研究沿起…………………………………8
2.3.2 多氯聯苯來源及生成機制……………………………8
2.3.3 多氯聯苯之特性…………………………………………9
2.3.4 多氯聯苯之危害………………………………………10
2.4 海洋沈積物品質參考準則…………………………………11
第三章 實驗設備與研究方法…………………………………………19
3.1 材料與儀器…………………………………………………19
3.1.1 材料…………………………………………………19
3.1.2 儀器…………………………………………………20
3.2 試藥及器材前處理…………………………………………20
3.3 採樣及樣品前處理…………………………………………21
3.4 多環芳香烴及多氯聯苯分析方法…………………………21
3.4.1 多環芳香烴及多氯聯苯分析方法流程………………21
3.4.2 多環芳香烴分析………………………………………21
3.4.3 多氯聯苯分析…………………………………………23
3.4.4 定量方法………………………………………………24
3.4.5 品保及品管（QA/QC）………………………………25
3.4.5.1 方法回收率……………………………………25
3.4.5.2 實驗空白分析與方法偵測極限……………26
3.5 顆粒有機碳（POC）分析…………………………………26
3.6 主成份分析（principal component analysis, PCA）…26
第四章 結果與討論……………………………………………………39
4.1 多環芳香烴化合物…………………………………………39
4.1.1 多環芳香烴之含量分佈………………………………39
4.1.2 總多環芳香烴濃度與文獻比較………………………40
4.1.3 總多環芳香烴濃度與總有機碳之相關性分析………41
4.1.4 多環芳香烴之來源……………………………………42
4.1.5 多環芳香烴之主成份分析(PCA)結果………………44
4.2 多氯聯苯化合物……………………………………………45
4.2.1 多氯聯苯之含量分佈…………………………………45
4.2.2 總多氯聯苯與文獻比較………………………………47
4.2.3 總多氯聯苯濃度與總有機碳之相關性分析…………48
第五章 結論與建議……………………………………………………85
5.1 結論…………………………………………………………85
5.2 建議…………………………………………………………87
參考文獻………………………………………………………89

表目錄
表2-1 US EPA 優先管制16種PAHs之理化性質……………………12
表2-2 16種PAHs之毒性特性…………………………………………13
表2-3 多氯聯苯之IUPAC命名………………………………………14
表2-4 多氯聯苯的主要用途…………………………………………16
表3-1 花蓮和平港港區與和平溪溪口採樣點經緯度與深度…………27
表3-2 四次分析樣品之PAHs擬似標準品回收率……………………28
表3-3 四次分析樣品之PCBs擬似標準品回收率……………………29
表3-4 四次分析樣品之PAHs標準品之回收率………………………30
表3-5 四次分析樣品之PCBs標準品之回收率………………………31
表3-6 四次分析樣品之PAHs之偵測極限……………………………33
表3-7 四次分析樣品之PCBs之偵測極限……………………………34
表4-1 四次採樣沈積物中多環芳香烴分析結果……………………49
表4-2文獻沈積物多環芳香烴濃度比較………………………………50
表4-3海洋沈積物品質參考標準與各採樣點平均PAHs值比較……51
表4-4 海洋沈積物品質參考標準與四次各採樣點總PAHs值比較…52
表4-5 四次採樣總有機碳分析結果…………………………………53
表4-6 四次採樣PAHs異構物比值……………………………………54
表4-7 主成份轉軸後之因素負荷表…………………………………55
表4-8 四次採樣沈積物中多氯聯苯總濃度分析……………………56
表4-9 四次採樣沈積物中多氯聯苯同源物分析結果………………57
表4-10 四次採樣各測站前三高濃度之多氯聯苯同源物……………60
表4-11 台灣地區沈積物多氯聯苯濃度比較…………………………61
表4-12 文獻沈積物多氯聯苯濃度比較………………………………62
表4-13 海洋沈積物品質參考標準與四次各採樣點總PCBs值比較………64

圖目錄
圖2-1 美國環保署列為16種優先處理的多環芳香烴結構式………17
圖2-2 多氯聯苯分子結構式…………………………………………18
圖3-1 花蓮和平港與和平溪溪口採樣點位置圖……………………37
圖3-2 樣品分析流程圖…………………………………………………38
圖4-1 四次採樣各採樣點總多環芳香烴平均含量……………………65
圖4-2 四次採樣沈積物中多環芳香烴總濃度分析……………………66
圖4-3 四個採樣點的沈積物中各多環芳香烴化合物分佈……………67
圖4-4 四次採樣各採樣點的沈積物中平均各多環芳香烴化合物之
百分比……………………………………………………………68
圖4-5四次採樣總PAHs濃度與沈積物品質指標比較………………69
圖4-6 總多環芳香烴與總有機碳線性關係……………………70
圖4-7 四次採樣各採樣點多環芳香烴特徵比（a）Phe/Ant vs Flth/Pry（b）Phe/Ant vs BaA/Chr………………………………………………71
圖4-8 四次採樣各採樣點多環芳香烴特徵比Flth/Flth+Pyr vs INP/INP+BghiP…………………………………………………72
圖4-9 四次採樣個別PAHs平均總濃度………………………………73
圖4-10 94年10月27日（秋季）各採樣點多環芳香烴含量………74
圖4-11 95年01月20日（冬季）各採樣點多環芳香烴含量………75
圖4-12 95年05月05日（春季）各採樣點多環芳香烴含量………76
圖4-13 95年08月16日（夏季）各採樣點多環芳香烴含量……77
圖4-14 PC1對PC2之因素分數圖…………………………………78
圖4-15 和平港與和平溪溪口之多環芳香烴相對濃度分佈…………79
圖4-16 四次採樣各採樣點總多氯聯苯平均含量……………………80
圖4-17 四次採樣沈積物中多氯聯苯總濃度分析……………………81
圖4-18 四次採樣總PCBs濃度與沈積物品質指標比較……………82
圖4-19 總多氯聯苯與總有機碳線性關係圖…………………………83

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