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研究生:陳凱亭
研究生(外文):kai-ting Chen
論文名稱:高雄港內水域多環芳香烴與多氯聯苯含量分佈
論文名稱(外文):Concentrations and distribution of polycyclic aromatic hydrocarbons(PAHs) and polychlorinated biphenyls(PCBs) in Kaohsiung Harbor
指導教授:李宗霖李宗霖引用關係
指導教授(外文):Chon-Lin Lee
學位類別:碩士
校院名稱:國立中山大學
系所名稱:海洋環境及工程學系研究所
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2010
畢業學年度:98
語文別:中文
論文頁數:206
中文關鍵詞:高雄港水氣交換通量多氯聯苯多環芳香烴
外文關鍵詞:Kaohsiung Harbor lagoonAir-water exchange fluxesPolychlorinated biphenyls (PCBs)Polycyclic aromatic hydrocarbons (PAHs)
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持久性有機污染物(Persistent Organic Pollutants, POPs)藉由水氣界面之傳輸作用對於此類化合物在全球環境中之分佈相當重要,本研究旨在延續前人對於高雄港區大氣及水中多環芳香烴(PAHs)之水氣交換通量(方,2007),前人研究是以單一測站之年度水氣交換通量視為高雄港區年度交換通量結果,考慮高雄港區PAHs濃度分佈不均勻,故本研究計算高雄港區內多個測站(n=7)之水氣交換通量以及每年由高雄港區輸出之PAHs質量,與前者之結果比較其差異性。本研究並探討高雄港港區水體懸浮顆粒相、溶解相中PAHs與PCBs含量、分佈與特性,以及沉積物中PAHs含量與分佈;並以化學指紋鑑定、群集分析、主成分分析判斷水體中PAHs可能污染來源。
 濕季海水總多環芳香烴濃度(47PAHs)分佈介於21.6-36.2 ng/L,平均濃度為28.2 ng/L,溶解相和顆粒相的濃度分別為15.5-27.2 ng/L以及3.4-8.6 ng/L。乾季海水總多環芳香烴濃度分佈介於13.2-31.5 ng/L,平均濃度為21.0 ng/L,溶解相和顆粒相的濃度分佈分別為8.0-21.1 ng/L以及5.3-10.5 ng/L,溼季總多環芳香烴濃度比乾季高,乾季以前鎮河河口的濃度最高,高雄港港區南端的測站濃度皆偏高,是因鄰近大林臨海工業區。沉積物總多環芳香烴濃度分佈介於81.7-2279 ng/g,平均濃度為895 ng/g。
探討有機碳、水溫、鹽度、懸浮顆粒濃度對多環芳香烴濃度的影響,乾季水溫對溶解相PAHs濃度有顯著負相關(p<0.05),沉積物PAHs濃度與總有機碳有顯著正相關(p<0.05),與顆粒之中值粒徑有顯著負相關(p<0.01)。乾濕季的logKoc與logKow與文獻logKoc-logKow方程式比較,截距均比其他地區高,可能是受到顆粒中soot顆粒的影響。
溼季溶解相屬於偏燃燒之混合來源,顆粒相則屬於偏石油之混合來源。乾季溶解相屬於偏石油之混合來源,且相對而言,南端測站石油污染風化程度較高,表示南端測站石油污染平均停留之時間比北端測站久,北端測站的石油污染可能一直有較多新污染輸入;乾季顆粒相屬於偏燃燒之混合來源。
濕季海水總多氯聯苯濃度分佈介於1.1–2.7ng/L,平均濃度為1.8ng/L,溶解相和顆粒相的濃度分別為0.42 –2.1 ng/L以及0.24–1.4 ng/L。乾季海水總多氯聯苯濃度分佈介於0.54–1.3 ng/L,平均濃度為0.98 ng/L,溶解相和顆粒相的濃度分佈分別為0.20–0.74ng/L以及 0.32–0.76 ng/L。
夏季(2008年7月)所有PAHs化合物之淨通量皆為正值,表示PAHs是由水相進入氣相中;冬季(2008年12月)四環以上PAHs如Fluoranthrene、Chrysene +Triphenylene、Benzo[a]anthracene之淨通量皆為負值,表示PAHs是由氣相進入水相中。本研究並比較以單一測站濃度與散佈於高雄港之測站平均濃度所計算水氣交換通量的不同,結果顯示若以單一測站計算通量可能會低估Pyrene的通量以及乾季的總通量。以高雄港區年度多環芳香烴淨通量(212mg/m2 /year)估計高雄港區每年由水中往大氣輸出多環芳香烴約5.7 kg。
This study investigated the concentrations of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) in the particulate and dissolved phase, as well as concentrations of PAHs in the sediment in Kaohsiung Harbor lagoon. Sources of PAHs in the water column were determined by isomer ratios, hierarchical cluster analysis (HCA) and principal components analysis (PCA). The net and annual fluxes of PAHs were calculated after a lagoon-wide water sampling campaign and compared with those found in a previous study (Fang, 2007) in which data from only one water sampling station was used.
  In rain season, total PAH concentrations ranged from 21.6 to 36.2 ng/L for water samples, with dissolved and particulate phase concentrations ranged from 15.5 to 27.2 ng/L and from 3.4 to 8.6 ng/L, respectively. In dry season, total PAH concentrations ranged from 13.2 to 31.5 ng/L for water samples, with dissolved and particulate phase concentrations ranged from 8.0 to 21.1 ng/L and from 5.3 to 10.5 ng/L, respectively. Total PAH concentrations were found higher in rain season than in dry season. The highest total PAH concentration in dry season was observed in Chianjen River estuary. Relatively high PAH concentrations were also observed in these southern stations of Kaohsiung Harbor because of their location near Dalin industrial park. Total PAH concentrations ranged from 81.7 to 2279 ng/g for sediment samples, with average of 895 ng/g.
The correlations between PAH concentrations and organic carbons, water temperature, salinity and suspended particles were also examined in this study. PAH concentration in dissolved phase was negatively correlated with water temperature (p&lt;0.05). PAH concentration in sediment was positively correlated with organic carbons (p&lt;0.05), and negatively correlated with median diameter (p&lt;0.01). The logKoc-logKow relationship in rain and dry season was compared with literature. It was found that the logKoc values were higher than those reported in literature, suggesting that soot particles might play an important role in the transport and distribution of PAHs in the study area.
In rain season, PAHs in dissolved phase were mainly from pyrogenic origins; while mainly from petrogenic origins in particulate phase. In contrast, in dry season, PAHs in dissolved phase were mainly from petrogenic origins; while mainly from pyrogenic origins in particulate phase. In addition, it was found, relatively, that petrogenic pollution was introduced maily from the northern area of the lagoon.
In rain season, total PCB concentrations ranged from 1.1 to 2.7 ng/L for water samples, with dissolved and particulate phase concentrations ranged from 0.42 to 2.1 ng/L and from 0.24 to 1.4 ng/L, respectively. In dry season, total PCB concentrations ranged from 0.54 to 1.3 ng/L for water samples, with dissolved and particulate phase concentrations ranged from 0.20 to 0.74 ng/L and from 0.32 to 0.76 ng/L, respectively.
The direction of net fluxes of PAHs in this study are from water to air (net volatilization) in summer. In winter, however, the absorptive PAH fluxes obtained for four to six-ring PAH, such as fluoranthrene, chrysene + triphenylene and benzo[a]anthracene, indicating that PAHs were absorbed into surface waters. According to our results, it was suggested that the results from previous study (Fang, 2007) might underestimate the net fluxes of Pyrene and total fluxes in dry season. The annual fluxes of PAHs estimated in this study were 212 mg/m2 /year and 5.7 kg of PAHs were emitted annually from the harbor lagoon surface waters to the ambient atmosphere.
摘要
Abstract
目錄 ……..…..I
圖目錄 ………..IV
表目錄 ….…….VI
附錄 .……..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持久性有機污染物(POPs) ...…….………………………………...……3
2-2多環芳香烴(PAHs)概述………………………………………………….9
2-2-1多環芳香烴及其物化特性.…………………………………...…9
2-2-2多環芳香烴之毒理特性………………………………………..13
2-2-3多環芳香烴之來源……………………………………………..15
2-2-4多環芳香烴之化學指紋鑑定…………………………………..16
2-3多氯聯苯(PCBs)概述………………………………………...……...…19
2-3-1多氯聯苯及其物化特性………………………………………..19
2-3-2多氯聯苯之毒理特性…………………………………………..24
2-3-3多氯聯苯之來源………………………………………………..24
2-4多環芳香烴與多氯聯苯之傳播途徑……………………………………26
2-5水氣交換通量…………………………………….……….............……28
2-6研究區域現況描述…………………………………….……………..…29
2-6-1氣候 …………………………………………….…………...…29
2-6-2海流流向 ……………………………………..………….....…29
2-6-3高雄港區可能污染來源.……………………..…...……..…….30
第三章 研究方法及步驟...………………………………………………...…31
3-1材料與儀器………………………………………………………………31
3-1-1材料……………………………………………………………..31
3-1-2儀器設備 ………………………………………………………32
3-1-3試藥及器材前處理 ……………………………………………33
3-2採樣之時間地點及方法 ………………………………………………34
3-2-1海水..……………………………………………………………39
3-2-2沉積物..…………………………………………………………39
3-2-3氣相..……………………………………………………………39
3-3多環芳香烴與多氯聯苯分析方法..……………………………...……40
3-3-1多環芳香烴(PAHs)分析..………………………………...……40
3-3-2多氯聯苯(PCBs)分析 .…………………………………...……45
3-3-3品保與品管(QA-QC) .…………………………………...……48
3-4有機碳分析方法 .…………………………………...…………………49
3-4-1水相顆粒相有機碳(POC)及溶解相有機碳(DOC)分析 .…….49
3-4-2沉積物有機碳(POC)分析 ……….……………………...…….50
3-5粒徑分析 .……………………………………………………...………50
3-6水氣交換 .……………………………………………………...………51
3-6-1水氣交換之模式(二層膜理論) ..………………………………51
3-6-2亨利常數 .………………………………………………………54
3-7群集分析(Hierarchical Cluster Analysis, HCA).…………………… 57
3-8主成分分析(Principal Components Analysis , PCA).…….…...……57
第四章 結果與討論…. ………………………………………………...……..58
4-1多環芳香烴(PAHs) ….………………………………………………….58
4-1-1海水及沉積物PAHs濃度分佈……………………….…………58
4-1-2沉積物中品質指標(Sediment Quality Guidelines, SQG)……67
4-1-3影響多環芳香烴濃度分佈之因子………………………………68
4-1-4 logKoc–logKow關係………………...……………………………73
4-1-5化學指紋鑑定 ……………………………………………………78
4-1-6群集分析 ……………………………...…………………………83
4-1-7主成分分析….……………………………………...……………90
4-2多氯聯苯(PCBs) ………………………..…………………………….100
4-2-1海水PCBs濃度分佈…………….………………………….…100
4-2-2影響多氯聯苯濃度分佈的因子 …….………………………….106
4-3水氣交換 ………….…………………………………………………….109
4-3-1水氣交換通量...……………………………...………………….109
4-3-2季節性以及年度水氣交換通量...……………………...……….124
4-3-3與其他地區比較水氣交換通量 ..…………………………...….128
第五章 結論與建議 ................................................................................130
5-1 結論 …………………………..……………………………...………..130
5-2 建議 ………………………..……………………………...…………..132
參考文獻…………………………………………………………...………….133
附錄 ……………………………………………...…………………………….142











圖目錄
圖2-1美國環保署所列16種優先處理之多環芳香烴..………….……………10
圖2-2多氯聯苯結構圖.…………………………………………………………19
圖2-3多環芳香烴在大氣、水以及土壤中之傳輸途徑.……………………..…27
圖2-4高雄港海域在(a)漲潮時;(b)退潮時之流場分佈………………….……30
圖3-1高雄港採樣位置圖 ………………………………………...……………35
圖3-2 2005-2007年雨量分佈圖…….…………………………………………35
圖3-3 (a)2008年7月;(b)2009年4月雨量圖…………………………………36
圖3-4 (a)2008年7月21日;(b)2009年4月30日水位資料…………..……..37
圖3-5海水樣品多環芳香烴(PAHs)分析流程示意圖.………………………...41
圖3-6沉積物樣品多環芳香烴(PAHs)分析流程示意圖.………………...…... 42
圖3-7多氯聯苯(PCBs)分析流程示意圖.……………………………....……..46
圖3-8水氣交界面示意圖.……………………………………………... .……..51
圖4-1 (a)濕季;(b)乾季 海水多環芳香烴濃度與懸浮顆粒濃度分佈圖..….…61
圖4-2 PAHs環數分佈…………………….………………………………….…62
圖4-3乾季溶解相 Pyrene 濃度分佈圖………………………………………63
圖4-4乾季溶解相Fl/Fl+Py比值…………………………………….…………63
圖4-5溶解相與顆粒相多環芳香烴環數分佈圖………………………….……64
圖4-6沉積物總多環芳香烴濃度分佈………………………………….………65
圖4-7乾季顆粒相多環芳香烴(PAHs)與有機碳(POC)之相關性分析…….....69
圖4-8溼季顆粒相多環芳香烴(PAHs)與有機碳(POC)之相關性分析…….....70
圖4-9 (a)沉積物多環芳香烴(PAHs)與有機碳(POC)之相關性分析
(b)沉積物多環芳香烴(PAHs)與中值粒徑大小之相關性分析 ………..72
圖4-10 (a)乾季;(b)濕季 logKoc-logKow關係圖…………..……...…….….….74
圖4-11溶解相指紋鑑定指標圖……………………………………….………..79
圖4-12顆粒相指紋鑑定指標圖…………………………………………….…..82
圖4-13溶解相群集分析…………………………………………………….…..84
圖4-14溶解相Cluster1、Cluster2和Cluster3多環芳香烴分佈圖…………..85
圖4-15乾季溶解相46DMD與36DMP比值.…………...………………….....86
圖4-16顆粒相群集分析………………………………………………………...88
圖4-17顆粒相Cluster1和Cluster2多環芳香烴分佈圖…………………..….89
圖4-18溶解相主成分分析:第一主成分loading圖…………………...………91
圖4-19溶解相主成分分析:第二主成分loading圖……………………...……92
圖4-20乾溼季顆粒相主成分分析分數圖PC1 – PC2 ……………………….93
圖4-21顆粒相主成分分析:第一主成分loading圖………………………...…96
圖4-22顆粒相主成分分析:第二主成分loading圖…………………...………97
圖4-23乾溼季顆粒相主成分分析分數圖PC1 – PC2 …..……………...……98
圖4-24 (a)濕季;(b)乾季 多氯聯苯濃度分佈圖……………………………..102
圖4-25乾溼季顆粒相多氯聯苯與有機碳之相關性…………………...…….107
圖4-26 (a)氣相;(b)溶解相 多環芳香烴濃度,以及(c)採樣當月雨量分佈....110
圖4-27採樣當日之風向風速玫瑰圖…………………...…..………………...111
圖4-28氣相、溶解相之Acenaphthylene濃度及水氣交換通量…………….113
圖4-29氣相、溶解相之Acenaphthene濃度及水氣交換通量……….…......114
圖4-30氣相、溶解相之Fluorene濃度及水氣交換通量………..…………....115
圖4-31氣相、溶解相之Phenanthrene濃度及水氣交換通量 …………..….116
圖4-32氣相、溶解相之Anthracene濃度及水氣交換通量 ………….…..…117
圖4-33氣相、溶解相之1-Methyphenanthrene濃度及水氣交換通量…..….118
圖4-34氣相、溶解相之Fluoranthene濃度及水氣交換通量……….…….…119
圖4-35氣相、溶解相之Pyrene濃度及水氣交換通量……….……..………..120
圖4-36氣相、溶解相之Benzo[a]anthracene濃度及水氣交換通量……..…121
圖4-37氣相、溶解相之Chrysene+Triphenylene濃度及水氣交換通量…...122
圖4-38 (a)乾季;(b)濕季水氣交換通量(ng/m2/day)……..………..……...…125
圖4-39年度水氣交換通量(ng/m2/year) ………..………..………....……….127
圖4-40年度蒸發通量以及吸收通量(ng/m2/year) ….….….…………….….128
表目錄
表2-1聯合國環境規劃署於1995年公告12種化學物質及我國管理現況.........4
表2-2 12種持久性有機污染物(POPs)毒性及致癌分類…………..…….………6
表2-3斯德哥爾摩公約於2005年建議增列16種持久性有毒物……..…..…….7
表2-4斯德哥爾摩公約於2007年增列之10種化合物及我國管理現況…….…8
表2-5本研究分析之多環芳香烴種類(47 PAHs) ………..………..……..……11
表2-6美國環保署所列之16種優先處理多環芳香烴之物理化學特性..….…12
表2-7國際組織對多環芳香烴致癌性之研究..………..………..……………..14
表2-8文獻中不同來源之多環芳香烴特徵比………..………..……...…….... 18
表2-9多氯聯苯IUPAC之命名………..………. …………..……….…...…….20
表2-10本研究之多氯聯苯種類(IUPAC no.) ……………….....…………..….21
表2-11多氯聯苯之物理化學特性………..………..…………..………..…..…22
表2-12多氯聯苯之主要用途………..………..…………..………..……..……25
表3-1水樣品採樣測站資訊以及命名………..………..……………………….38
表4-1溶解相之多環芳香烴濃度(ng/L)與其他文獻比較 ……..…..….………59
表4-2海水之phenanthrene與pyrene總濃度(ng/L)與其他文獻比較………60
表4-3沉積物之多環芳香烴總濃度與文獻比較………………………..…….. 66
表4-4沉積物中品質指標(SQG)與樣品百分比.............................................67
表4-5溶解相多環芳香烴之相關係數矩陣圖………………………………….67
表4-6乾季顆粒相多環芳香烴(PAHs)與有機碳(POC)之比值…………….…69
表4-7溼季顆粒相多環芳香烴(PAHs)與有機碳(POC)之比值…………….…71
表4-8沉積物之粒徑分析(μm)………………………………………………….72
表4-9乾溼季各測站多環芳香烴的logKoc值……………………………….…75
表4-10乾濕季各測站多環芳香烴的logKoc值與文獻比較…………………...77
表4-11溶解相化學指紋鑑定、群集分析以及主成分分析結果…………….…94
表4-12顆粒相化學指紋鑑定、群集分析以及主成分分析結果……….……...99
表4-13與其他文獻多氯聯苯比較…………………………………….………103
表4-14溶解相與顆粒相不同氯數多氯聯苯之濃度分佈及佔總濃度百分比.104
表4-15 Weight % in Aroclors .………….……….………………….……..…105
表4-16溶解相多氯聯苯之相關係數矩陣圖………………….……….……. 106
表4-17顆粒相多氯聯苯之相關係數矩陣圖………. ………. ……..………. 108
表4-18多環芳香烴之水氣交換通量(ng/m2/day) ……………………..….…123
表4-19 phenanthrene及pyrene通量(ng/m2/day)與其他地區比較............129
























附錄
附錄I-1各測站添加PAHs擬似標準品回收率(%)………..…...………..……A-1
附錄I-2各測站添加PCBs擬似標準品回收率(%)…………….………..……A-3
附錄I-3乾季溶解相多環芳香烴空白分析及偵測極限(pg/L) ………..…...…A-5
附錄I-4溼季溶解相多環芳香烴空白分析及偵測極限(pg/L) ……………….A-6
附錄I-5乾季顆粒相多環芳香烴空白分析及偵測極限(pg/L) ………..…...…A-7
附錄I-6溼季顆粒相多環芳香烴空白分析及偵測極限(pg/L) ……….………A-8
附錄I-7沉積物多環芳香烴之偵測極限(pg) ……….…….……….……….…A-9
附錄I-8溶解相多氯聯苯之偵測極限(pg/L)…………………..………….....A-10
附錄I-9顆粒相多氯聯苯之偵測極限(pg/L) ..……….………..………..…...A-12
附錄I-10水樣添加51PAHs樣品之回收率(%) ...……….…………...…….A-14
附錄I-11沉積物之標準查核分析(SRM) ..………..……..………..………...A-15
附錄II-1溼季溶解相濃度(ng/L) ..……….………..…………………..………B-1
附錄II-2乾季溶解相濃度(ng/L) ....…….…..………..………..………..…..…B-2
附錄II-3溼季顆粒相濃度(ng/L) ..………..……..……..………..…………….B-3
附錄II-4乾季顆粒相濃度(ng/L) ..……….……….…………….………..……B-4
附錄II-5溼季顆粒相濃度(ng/g) .…………………..………..…. ……………B-5
附錄II-6乾季顆粒相濃度(ng/g) ..………..………..………..……..….………B-6
附錄II-7沉積物多環芳香烴濃度(ng/g) ..………..……....…………...………B-7
附錄II-8有機碳濃度……………………..………..……….………..…….…..B-8
附錄II-9溶解相主成份分析之成分矩陣..………..……….………..………...B-9
附錄II-10顆粒相主成份分析之成分矩陣….…….…………..………....…..B-10
附錄II-11溼季溶解相PCBs濃度(pg/L) …..………..……..………………...B-11
附錄II-12乾季溶解相PCBs濃度(pg/L)...….…….………...…………….…B-13
附錄II-13溼季顆粒相PCBs濃度(pg/L) …………..……….………..……..B-15
附錄II-14乾季顆粒相PCBs濃度(pg/L) .………. ………..………..……….B-17
附錄II-15溼季顆粒相PCBs濃度(ng/g) ..………. ………..……….……….B-19
附錄II-16乾季顆粒相PCBs濃度(ng/g) ..………….……..………..……....B-21
附錄II-17 Co-Eluting 多氯聯苯同源物在不同同族物之間分配比例. ……B-23
附錄II-18乾濕季溶解相多氯聯苯之相關係數矩陣圖…………....………..B-24
附錄II-19乾濕季顆粒相多氯聯苯之相關係數矩陣圖.……..…….….........B-25
附錄II-20 2008以及2009年每月雨量分佈圖……….……..…….………..B-26
附錄II-21根據每小時風向風速繪製每月之風向風速玫瑰圖..………..…..B-27
附錄II-22水氣交換數據. ………..………..………..………..…….…..…….B-30
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