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博碩士論文 etd-1129112-133846 詳細資訊
Title page for etd-1129112-133846
論文名稱
Title
多環芳香烴於高屏海域水體中含量分佈
Distribution of polycyclic aromatic hydrocarbons (PAHs) in Gao-ping coastal water column
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
197
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2012-11-26
繳交日期
Date of Submission
2012-11-29
關鍵字
Keywords
多環芳香烴、高屏海域、溶解相、顆粒相、沉積物
PAHs, Gao-ping coast, dissolved phase, particulate phase, sediment
統計
Statistics
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The thesis/dissertation has been browsed 5754 times, has been downloaded 6 times.
中文摘要
本研究主要分析高屏海域水體(溶解相及顆粒相)與高屏峽谷沉積物的多環芳香烴(PAHs)濃度,採樣時間為2010年8、11月及2011年2、6月,從高雄港近岸至高屏溪出海口,距離岸邊2公里至15公里處分層水域水體與高屏峽谷沉積物,探討在空間及季節上變化的分佈情形與可能影響的因素,加上以化學指紋鑑識(chemical fringer printing)、主成分分析(principal component analysis, PCA)與群集分析(hierarchical cluster analysis, HCA)推測多環芳香烴的可能來源,並透過鹽度、溫度與有機碳百分比等作相關性分析。
研究結果顯示在四次採樣海域多環芳香烴總濃度(溶解相+顆粒相)介於2.09~45.0 ng/L間。溶解相多環芳香烴的總濃度變化為2.0~39.0 ng/L,以2010年11月份10.0±9.90 ng/L(1.96~39.0 ng/L)為四次採樣中有最高的平均濃度;顆粒相多環芳香烴總濃度介於0.13~40.0 ng/L間,峰值發生於2010年8月河口地區或河口地區延伸處底層,本研究海域多環芳香烴濃度普遍低於文獻測值;沉積物多環芳香烴總濃度介於125~648 ng/g間,樣品濃度均低於ERL與TEL值,不易對峽谷生物產生顯著影響。
從指紋分析、主成分分析與群集分析上可以得知研究區域的多環芳香烴屬於複雜性的來源,如燃燒性來源、石油性來源、成岩作用或生物來源等。溶解相多以石油/混合來源為主、顆粒相多以混合來源為主,於2010年11月與2011年2月樣品可能受到大氣影響,多偏向混合/燃燒來源。高屏海域與高屏峽谷perylene可能多來自生物來源。河口地區底層水顆粒相與沉積物顯著相關,表示河口輸出物質可能會形成峽谷沉積物之來源。
在多環芳香烴相關性分析上,海域顆粒相多環芳香烴與懸浮顆粒濃度具顯著相關性;與溫度呈現顯著的負相關。峽谷沉積物的有機碳含量百分比與多環芳香烴有顯著相關。在Log Koc與 Log Kow關係上截距均高於文獻值,可能受到河口輸出soot carbon影響。
Abstract
Water, suspended particle and sediment samples from Gao-ping coastal water column were collected and measured to determine the spatial and temporal distributions of polycyclic aromatic hydrocarbons (PAHs) during August 2010 and June 2011. In addition, principal component analysis (PCA) and hierarchical the cluster analysis (HCA) were performed with chemical fingerprinting to understand the possible sources of PAHs in Gao-ping coast. The correlations between PAHs and several factors such as salinity, temperature and organic carbon were also discussed in the present study.
The total PAH concentrations (dissolved and particulate phase) at four sampling campaigns ranged from 2.09 to 45 ng/L. Concentrations of dissolved PAHs ranged from 2.0 to 39 ng/L and the highest average concentrations were found in November 2010 (10.0 ± 9.90 ng/L). The particulate PAHs ranged from 0.13 to 40 ng/L and the maximum concentration was found in the estuary in August 2010. The total PAH concentrations of sediment ranged from 125-648 ng/g, which were lower than the Effect Range Low (ERL) and Threshold Effect Level (TEL) values, suggesting that few adverse ecological effects would arise from the PAHs in Gao-ping canyon.
Results from chemical fingerprinting, PCA and HCA indicate that PAHs in this area were from complex sources such as combustion, petroleum, diagenesis or biogenic sources. Sources of PAHs in dissolved phase were mainly from petrogenic and mixed sources, while particulate PAHs were mainly from a mixed source. However, sources of PAHs in November 2010 and February 2011 were mostly from mixed combustion, suggesting that the PAH concentrations in particulate phase might be affected by atmospheric transport. The results showed that perylene in Gao-ping coast and canyon was mainly from the biogenic source. A significant correlaction was found in PAH fingerprinting between the esturine particles and sediment, indicating that the sediments in Gao-ping canyon might mainly come from Gao-ping River.
Correlation analysis showed a significant positive correlation between concentrations of suspended particle and PAHs, while a negative correlation was found between PAH concentrations and temperature. In addition, organic carbon showed a significant correlation with PAHs in sediment samples. The partition coefficients (Koc) values of PAHs were higher than the values from other literatures, suggesting that it might be attributed to soot carbon.
目次 Table of Contents
謝誌 i
摘要 ii
Abstrat iv
目錄 vi
圖目錄 ix
表目錄 xi
附錄目錄 xi
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 多環芳香烴的特性 3
2-2 多環芳香烴來源 7
2-3 毒性 8
2-4 多環芳香烴的化學指紋鑑識 8
2-5 高屏海域 10
2-5-1 地理特性 10
2-5-2 高屏海域之流場 10
2-5-3 高屏海域沿岸特色 11
2-6群集分析 (hierarchical cluster analysis, HCA) 12
2-7 主成分分析 (principle component analysis, PCA) 12
2-8 沉積物的應用 13
第三章、研究方法與實驗 14
3-1 實驗材料與儀器 14
3-1-1 材料 14
3-1-2 儀器 15
3-2 試藥及器材前處理 15
3-3 採樣與保存 17
3-3-1 採樣點位 17
3-3-2 採樣方法 19
3-4 實驗分析方法 20
3-4-1 海水溶解態樣品分析 20
3-4-2 海水顆粒態樣品分析 21
3-4-3 沉積物樣品分析 21
3-5 分析定量 21
3-6 品管及品保(QA/QC) 22
第四章 結果與討論 25
4-1 高屏海域溶解相多環芳香烴 25
4-1-1 溶解相多環芳香烴總濃度分佈 25
4-1-2 表層水多環芳香烴總濃度 28
4-1-3 表層水和底層水總濃度分佈 31
4-1-4 溶解態環數分佈 35
4-2 高屏海域顆粒相多環芳香烴 38
4-2-1 顆粒相多環芳香烴總濃度分佈 38
4-2-2 顆粒相多環芳香烴環數百分比分佈 44
4-3 高屏峽谷沉積物多環芳香烴 47
4-3-1總濃度分佈 47
4-3-2 沉積物多環芳香烴相關性分析 52
4-4 來源判定分析 53
4-4-1 溶解相多環芳香烴化學指紋特徵 53
4-4-2 溶解相多環芳香烴主成分分析 56
4-4-3 溶解相多環芳香烴群集分析 60
4-4-4 顆粒相多環芳香烴化學指紋特徵 63
4-4-5 顆粒相多環芳香烴主成分分析 68
4-4-6 顆粒相多環芳香烴群集分析 72
4-4-7 沉積物多環芳香烴化學指紋特徵 75
4-4-8 沉積物多環芳香烴主成分分析 78
4-4-9 沉積物多環芳香烴群集分析 81
4-5 Perylene 來源探討 84
4-5-1 高屏海域顆粒相perylene來源 84
4-5-2 高屏峽谷沉積物 perylene來源 87
4-6 文獻比較 89
4-6-1 海域溶解態多環芳香烴總濃度文獻比較 89
4-6-2 海域顆粒相多環芳香烴總濃度文獻比較 91
4-6-3 沉積物多環芳香烴總濃度文獻比較 93
4-6-4 沉積物品質指標 (Sediment Quality Guidelines, SQG) 96
4-7 高屏海域水體與峽谷沉積物多環芳香烴之比較 100
4-7-1 顆粒相與沉積物多環芳香烴總濃度比較 100
4-7-2 峽谷沉積物與海域溶解相、顆粒相環數比較 102
4-7-3 海域顆粒相與峽谷沉積物之化學指紋比較 104
4-7-4 顆粒相與沉積物之主成分分析比較 106
4-8 多環芳香烴影響因子相關性分析 110
4-8-1 溶解相與顆粒相多環芳香烴相關性分析 110
4-8-2 海域水體多環芳香烴與有機碳相關分析Log Koc與 Log Kow 112
第五章 結論與建議 118
5-1 結論 118
5-2 建議 120
參考文獻 121
附錄 128
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