(3.236.118.225) 您好!臺灣時間:2021/05/16 10:39
字體大小: 字級放大   字級縮小   預設字形  
回查詢結果

詳目顯示:::

我願授權國圖
: 
twitterline
研究生:陳美華
研究生(外文):Mei-Hua Chen
論文名稱:油污染鑑識生物指標技術應用研究-檢測流程與統計分析之應用與探討
論文名稱(外文):Study of biomarker and diagnostic ratio approaches for oil spill identification- application of modified oil spill identification flowchart with multivariate statistical analysis techniques
指導教授:高振山高振山引用關係吳素慧吳素慧引用關係
指導教授(外文):Chen-Shan KaoSuh-Huey Wu
口試委員:沈俊卿郭政隆
口試委員(外文):Jun-Chin ShenCheng-Lung Kuo
口試日期:2011-06-15
學位類別:碩士
校院名稱:國立聯合大學
系所名稱:環境與安全衛生工程學系碩士班
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:2011
畢業學年度:99
語文別:中文
論文頁數:211
中文關鍵詞:油污染鑑識;生物指標;統計分析;原油;柴油
外文關鍵詞:Oil spill identificationboimarkerstatistical approachcrude oildiesel
相關次數:
  • 被引用被引用:4
  • 點閱點閱:421
  • 評分評分:
  • 下載下載:0
  • 收藏至我的研究室書目清單書目收藏:1
本研究首先針對不同地區與國家之原油,使用油品化學指紋圖譜配合具來源意義特徵因子比值之鑑定技術,分析各種原油間之差異性,並藉由已知來源地區原油的特徵因子比值特性,刪去易造成誤差的比值。研究中藉由分析比對過程找出適用的生物指標與來源特徵性較高之比值,建立合適的油污染鑑識流程圖,並依此推測未知地區進口原油特性。研究進一步將此流程應用於鑑識不同煉製方法之柴油,分析探討不同煉製方法對油品特性之影響,找出柴油鑑識適用的生物指標與特徵因子比值。鑑識流程中配合多元統計方法(如PCA、HCA),利用其具備同時對多種比值進行分析的特點,快速有效的將油品分群並探討特徵因子比值選取對其分群效果之影響。並進一步運用重覆性限法與t檢驗評估圖分析技術,針對經由傳統一般指紋圖譜比對方法與多元統計方法尚無法鑑別的相似油品,進行評估以提供可信的佐證,並找出適用的特徵因子比值。本研究所建立之油污染鑑識流程與統計分析方法以及所適用的生物指標與特徵因子比值,當漏油事件發生時,將可作為確認漏油污染物的類型及追蹤污染源之有效工具。
Oil source tracking and identification related technologies are constantly being developed and applied since oil spill accidents occurred frequently that cause great impact on the environmental and ecological systems as well as the economy.
In this study, fresh crude oils from different regions and countries were analyzed and recognized by using chemical fingerprint chromatogram together with source-sensitive diagnostic ratios. Following the proposed oil spill identification flowchart with various appropriate biomarkers and source-specific ratios, it’s possible to identify characteristics of crude oils from unknown resources. Moreover, oil characteristics can be classified even more effectively by multivariate statistical approach such as principal component analysis (PCA), hierarchical cluster analysis (HCA), repeatability limit and student’s t-test to statistically evaluate the imperceptible differences between oils.
It was shown that our proposed flowchart of oil spill identification with appropriate biomarkers and diagnostic ratios along with the multivariate statistical analysis techniques were also applied effectively to identify different diesel types, oil-to-oil correlation, and oil source tracking.

致謝 I
摘要 II
Abstract III
目錄 IV
圖目錄 VI
表目錄 XIII
第一章 前言 1
1-1研究背景 1
1-1-1環境法醫學 1
1-1-2油輪漏油事件 2
1-1-3其它漏油事件 5
1-1-4我國漏油污染事件 5
1-1-5我國相關法規 7
1-2研究動機 7
1-3研究目的 8
第二章 文獻回顧 9
2-1漏油污染檢測方法 9
2-2風化作用影響評估 12
2-3生物指標 15
2-3-1正烷烴 15
2-3-2異戊間二烯(Isoprenoids) 15
2-3-3生物指標定義 16
2-3-4生物指標化合物 16
2-4生物指標化合物分析方法 24
2-4-1分析方法 24
2-4-2特徵因子比值(Diagnostic Ratio, DR) 26
2-5油品指紋統計分析鑑別方法 30
2-5-1重覆性限法(Repeatability Limit) 30
2-5-2 t檢驗方法(Student’s t-test) 30
2-5-3集群分析法(Cluster Analysis) 31
2-5-4主成份分析法(Principal Component Analysis, PCA) 32
2-6 國內外相關研究文獻之探討 33
2-7 漏油污染鑑識評估 43
第三章 材料與方法 44
3-1油污染鑑識流程 44
3-2實驗藥品與材料 44
3-3氣相層析質譜儀 (GC/MS) 48
3-3-1 GC/MS分析設定 48
3-3-2氣相層析質譜分析-離子源 48
3-4油品生物指標之定性描述 50
3-5上機條件分析 65
3-6特徵因子比值計算與一致性評估 71
3-6-1特徵因子比值計算 71
3-6-2特徵因子比值對比分析 71
3-6-3樣品一致性(Match)評估 72
第四章 結果與討論 75
4-1進口原油生物指標指紋圖譜分析 75
4-2使用原油分析具來源特徵性(Source-Sensitive)的特徵因子比值 107
4-3原油特徵因子比值之對比分析 111
4-4原油特徵因子比值一致性(Match)評估 131
4-5煉製油品生物指標指紋圖譜分析 148
4-6柴油特徵因子比值計算與評估 166
4-7柴油特徵因子比值之對比分析 168
4-8柴油特徵因子比值一致性(Match)評估 175
第五章 結論與建議 181
5-1結論 181
5-2建議 182
參考文獻 183

1.許信豐,「臺灣近代湖泊沉積物所含生物指標的分佈與其意義」,國立中山大學化學系研究所,碩士論文,1990。
2.韓蕙如,「凝結油中芳香烴的組成及來源分析」,國立成功大學化學系研究所,碩士論文,1994。
3.中華民國行政院環境保護署,「海洋污染防治法」,環保法規,2000。
4.孫培豔、高振會、崔文林,「油指紋鑒別技術發展與應用」,北京海洋出版社,2007。
5.中華民國行政院環境保護署,「土壤及地下水污染整治法」,環保法規,2003。
6.林國安、紀文榮、胡錦城、郭政隆、吳素慧、林麗華、沈俊卿,「石油探採(第一冊)-生油巖之油氣巖對比」,中國石油股份有限公司訓練教材叢書,212–240,2003。
7.張小萍,「環境污染物指紋資料庫在環境管理上之應用」,環境檢驗第50期,22–26,2004。
8.吳素慧、郭政隆、林政遠、孫智賢,「芳香烴在台灣西部第三紀生油巖對比上之應用」,中國石油股份有限公司探採研究所,九十二年度研究報告,2003。
9.陳郁仁,「整治復育技術:國內土壤及地下水整治技術相關研究彙整~柴油」,環保技術e報第21期,2004。
10.蘇意筠、張祖恩,「我國環境法醫之發展現況與展望」,工業污染防治第93 期,77–98,2005。
11.吳素慧、高振山、吳姿燕、楊宗翰、陳美華,「海域油污染生物指標檢測技術建立(2/2)」,台灣中油公司探採研究所,98年度行政院環保署環境檢驗所委辦專案研究計畫報告,2009。
12.Alexander R., Kagi R. I., and Sheppard P.N.,「Relative abundance of dimethynaphthalene iaomers in crude oils」, Journal of Ghromatorgraphy, 267, 67–72 , 1983.
13.Aquino Neto F. R., Trendel, J. M., Restle, A., Connan, J., and Albrecht, P.A., 「Occurrence and formation of tricyclic and tetracyclic terpanes is sediments and petroleums」, In Advances in Organic Geochemistry 1981 (M. Bjoroy et al., eds) John Wiley and Sons, New York, p. 659–676, 2002.
14.Barakat A.O.,「Compositional change of aromatic steroid hydrocarbons in naturally weathered oil residues in the Egyptian western desert」, Environmental Forensics, 3, 219–225, 2002.
15.Boon J. J., Hine S. H., and Burlingame A. L.,「Organic geochemical studies of Solar Lake laminated cyanobacterial mats」, In Advances in Organic Geochemistry 1981, John Wiley and Sons, New York, 207–227, 1983.
16.Burgher P., 「In–depth analysis of accidental oil spills from tankers in the context of global spill trends from all sources」, Journal of Hazardous Materials, 140, 245–256, 2007.
17.CEN, 「European Committee for Standardization, Oil Spill Identification — Waterborne Petroleum and Petroleum Products — Part 2: Analytical Methodology and Interpretation of Results」, TC/BT TF 120 WI CSS27003, 2006.
18.Chosson P., Connan J., Dessert D., and Lanau C., 「 In vito biodegradation of steranes and terpanes: A clue to understanding geological situation. In Biological Markers in Sediments and Petroleum, edited by Moldowan et. al.」, Englewood Cliffs, NJ: Prentice Hall , 320–349 , 1992.
19.Daling Per S., Faksness Liv-Guri, Hansen Asger B., and Stout Scott A.,「Improved and standardized methodology for oil spill fingerprinting」, Environmental Forensics, 3, 263–278, 2002.
20.Diez Serggi , Jover Eric, Ayona Josep M. B , and Lbaiges Joan A, 「Prestige Oil Spill. III. Fate of a Heavy Oil in the Marine Environment」, Environ. Sci. Technol. 41, 3075–3082, 2007.
21.Douglas Gregory S., Bence A. Edward, Prince Roger C., McMillen Sara J., and Butler Eric L.,「Environmental Stability of Selected Petroleum Hydrocarbon Source and Weathering Ratios」, Environ. Sci. Technol., 30, 2332–2339, 1996.
22.Douglas Gregory S., Emsbo-Mattingly Stephen D., Stout Scott A., Uhler Allen D., and McCarthy Kevin J.,「Introduction to environmental forensics, Chapter 9, chemical fingerprinting methods」, Academic Press, 2007.
23.Ezra Shai, Feinstein Shimon, Pelly Ithamar, Bauman Dan, and Miloslavsky Irena,「Weathering of fuel oil on the east Mediterranean coast, Ashdod, Israel」, Organic Geochemistry 31, 1733–1741, 2000.
24.Faksness Liv-Guri, Weiss Hermann M., and Daling Per S.,「Revision of the Nordtest Methodology for Oil Spill identification」, SINTEF Applied Chemistry., NORWAY, 2002.
25.Fan P., Philp R.P., Zhenxi L., and Guangguo Y., 「Geochemical characteristics of aromatic hydrocarbons of crude oils and source rocks from different sedimentary environments」,Organic Geochemistry, 16, 427–435, 1990.
26.Ferna′ndez-Varela R., Andrade J.M., Muniategui S., Pradaa D., and Ramı′rez-Villalobos F.,「The comparison of two heavy fuel oils in composition and weathering pattern, based on IR, GC-FID and GC–MS analyses: Application to the Prestige wreckage」, Water Research 43, 1015–1026, 2009.
27.Garrett R.M., Pickering I.J., Haith C.E., and Prince R.C., 「Photooxidation of crude oils」, Environ. Sci. Technol. 32, 3719–3723, 1998.
28.Hughes W. B., Holba A. G., and Dzou L. I. P.,「The ratios of dibenzothiophene to phenanthrene and pristane to phytane as indicators of depositional environmental and lithology of petroleum source rock」, Geochim. Cosmochim. Acta 59, 3581–3598, 1995.
29.ITOPF,「Oil Tanker Spill Statistic:2009」, 2010.
30.Jonge H. de, Freijer J. I., Verstraten J. M., and Westerveld J., 「Relation between bioavailability and fuel oil hydrocarbon composition in contaminated soils」, Environ. Sci. Technol., 31,771–775, 1997.
31.Kaplan Isaac R., Galperin Yakov, Alimi Hossein, Lee Ru-Po, and Lu Shan-Tan, 「Patterns of Chemical Changes During Environmental Alteration of Hydrocarbon Fuels」, Ground Water Monitoring & Remediation, 113–125, 1996.
32.Li Yun, Xiong Yongqiang, Yang Wanying, Xie Yueliang, Li Siyuan, and Sun Yongge, 「Compound-specific stable carbon isotopic composition of petroleum hydrocarbons as a tool for tracing the source of oil spills」, Marine Pollution Bulletin 58, 114–117, 2009.
33.Malmquist Linus M.V., Olsen Rasmus R., Hansen Asger B., Andersen Ole, and Christensen Jan H.,「Assessment of oil weathering by gas chromatography–mass spectrometry, time warping and principal component analysis」, Journal of Chromatography A, 1164, 262–270, 2007
34.Marcio M. Lobao, Jari N. Cardoso, Marcio R. Mello, Paul W. Brooks, Claudio C. Lopes, and Rosangela S.C. Lopes, 「Identification of source of a marine oil-spill using geochemical and chemometric techniques」 , Marine Pollution Bulletin, 60 ,12, 2263–2274, 2010.
35.Michel Jacqueline, and Hayes Miles O., 「Weathering Patterns of Oil Residues Eight Years after the Exxon Valdez Oil Spill」, Marine Pollution Bulletin, 38, 10, 855–863, 1999.
36.Moldowan J.M., Steifert, W.K, and Gallegos, E.J.,「Relationship Between Petroleum Composition and Depositional Environment of Petroleum Source Rocks」, American Association of Petroleum Geologists Bulletin, 69, 8, 1255–1268, 1985.
37.Moldowan J. M., Lee C. Y., Sundararaman P., Salvatorl T., Alajbeg A., Gjukc B., and Demaison G. J.,「Source correlation and maturity assessment of select oils and rocks from the Central Adriatic Basin (Italy and Yugoslavia). In Biological Markers in Sediments and Petroleum, edited by Moldowan et. al.」, Englewood Cliffs, NJ: Prentice Hall, 370–401, 1992.
38.Murphy B. L., and Morrison R. D., 「Introduction to Environmental Forensics」, A Harcourt Science and Technology Company. p.148, 2002.
39.Noble R. A,「A geochemical study of bicyclic alkanes and diterpenoid hydrocarbons in crude sediments and coals」, Ph. D. thesis, Department of Organic Chemistry, University of Western Australia, Perth, Australia, 1986.
40.Oudot J, and Chaillan F.,「Pyrolysis of asphaltenes and biomarkers for the fingerprinting of the Amoco-Cadiz oil spill after 23 years」, Comptes Rendus Chimie, 13, 548–552, 2010.
41.Peters K. E., Walters C. C., and Moldowan J. M.,「The Biomarker Guide:Second Edition I. Biomarkers and Isotopes in the Environment and Human History」, Cambridge University Press, 2005.
42.Peters K. and Moldowan. J.M.,「The Biomarker Guide: Interpreting Molecular Fossils in Petroleum and Ancient Sediments」, Prentice Hall, New Jersey, 1993.
43.Prince R. C., Elmendorf D. L., Lute J.R., Hsu, C.S., Haith, C.E., Senius, J.D., Dechert, G.J., Douglas, G.S., and Butler, E.L., 「17a(H),21b(H)-hopane as a conserved internal marker for estimating the biodegradation of crude oil」 , Environ. Sci. Technol. 28, 142–145, 1994.
44.Prince Roger C., Owens Edward H., and Sergy Gary A., 「Weathering of an arctic oil spill over 20 years: the BIOS experiment revisited」, Marine Pollution Bulletin, 44, 1236–1242, 2002.
45.Qimin M.A., Zhanglin N.I., and Zhigang Y.U., 「The Biomarker Changes of a Heavy Fuel Oil After Different Weathering Times」, Oceanic and Coastal Sea Research, 8, 51–56, 2009.
46.Radke M., Willsch H., and Leythaeuser D.,「Aromatic components of coal: relation of distribution pattern to rank」, Geochimica et Cosmochimica Acta, 46, 1831–1848, 1982.
47.Short Jeffrey W., Irvine Gail V., Mann Daniel H., Maselko Jacek M., Pella Jerome J., Lindeberg Mandy R., Payne James R., Driskell William B., and Rice Stanley D., 「Slightly Weathered Exxon Valdez Oil Persists in Gulf of Alaska Beach Sediments after 16 Years」 , Environ. Sci. Technol., 41, 1245–1250, 2007.
48.Sun P., Bao M., Li G., Wang X., Zhao Y., Zhou Q., and Cao L., 「Fingerprinting and source identification of an oil spill in China Bohai Sea by gas chromatography-flame ionization detection and gas chromatography–mass spectrometry coupled with multi-statistical analyses」, Journal of Chromatography A, 1216, 830–836, 2009a.
49.Sun P., Gao Z., Zhou Q., Zhao Y., Wang X., Cao X., and Li G., 「Evaluation of the Oil Spill Accident in Bohai Sea, China」, Environmental Forensics, 10, 308–316, 2009b.
50.Tissot B.P, and Weldt D. H,「Petroleum Formation and Occurrence, 2nd Edition」, Springer-Verlag, New York, 393–408, 1984.
51.Vendeuvre Colombe , Ruiz-Guerrero Rosario , Bertoncini Fabrice , Duval Laurent , Thi′ebaut Didier ,and Hennion Marie-Claire, 「 Characterisation of middle-distillates by comprehensive two-dimensional gas chromatography (GC×GC): A powerful alternative for performing various standard analysis of middle-distillates」, Journal of Chromatography A, 1086, 21–28, 2005.
52.Volkman J. K., Alexander R., Kagi R.I., Rowland S. J., and Sheppard P. N.,「Biodegradation of aromatic hydrocarbons in crude oils from the Barrow sub-basin of Western Australia」, Organic Geochemistry 6, 619–632, 1984.
53.Wang Zhendi, and Fingas Merv,「Development of oil hydrocarbon fingerprinting and identification techniques」, Marine Pollution Bulletin 47, 423–452, 2003.
54.Wang Zhendi , and Fingas Merv,「Differentiation of the source of spilled oil and monitoring of the oil weathering process using gas chromatography-mass spectrometry」, Journal of Chromatography A, 712 , 321–343,1995a.
55.Wang Z. , and Fingas M., 「Study of the Effects of Weathering on the Chemical Composition of a Light Crude Oil Using GC/MS GC/FID」, J. Microcolumn Separations, 7, No.6,617–339 , 1995b.
56.Wang Z. , Fingas M., and Page D. S., 「Oil spill identification」, Journal of Chromatography A, 843 , 369–411, 1999.
57.Wang Z., and Stout A.S., 「Oil Spill Environmental Forensics: Fingerprinting and Source Identification: fingerprinting and source identification」, 2007.
58.Wang Z., Yang C., Hollebone B., and Fingas M.,「Forensic Fingerprinting of Diamondoids for Correlation and Differentiation of Spilled Oil and Petroleum Products」, Environ. Sci. Technol., 40, 5636–5646, 2006.
59.Wang Z., Yang C., Fingas M., Hollebone B., Peng X., Hansen A. B., and Christensen J.,「Characterization, Weathering, and Application of Sesquiterpanes to Source Identification of Spilled Lighter Petroleum Products」, Environ. Sci. Technol., 39, 8700–8707, 2005.
60.Wang Z., Yang C., Hollebone B., Brown C., and Landriault M.,「Source Identification of Spilled Diesel Using Diagnostic Sesquiterpanes and Diamondoids」, International Oil Spill Conference, 2008.
61.Williams J. A., Bjoroy M., Dolcater, D. L., Winters, J. C. ,「Biodegradation in South Texas Eocene oils-effects on aromatics and biomarkers」, Organic Geochemistry, 10, 451–461 ,1986.
62.Yang C., Wang Z., Hollebone B., Brown C.E., and Landriault M., 「Application of statistical analysis in the selection of diagnostic ratios for forensic identification of an oil spill source」, International oil spill conference, 2008.
63.Yang C., Wang Z., Hollebone B., Brown C.E., and Landriault M., 「Characteristics of bicyclic sesquiterpanes in crude oils and petroleum products」, Journal of Chromatography A, 1216, 4475–4484, 2009.
64.Zakaria Mohamad Pauzi, Horinouchi Ai, Shinobu Tsutsumi, Takada Hideshige, Tanabe Shinsuke, and Ismail Ahmad,「Oil pollutions in the straits of Malacca, Malaysia: Application of molecular markers for source identification」, Environ. Sci. Technol. 34, 1189–1196, 2000.

QRCODE
 
 
 
 
 
                                                                                                                                                                                                                                                                                                                                                                                                               
第一頁 上一頁 下一頁 最後一頁 top